diff --git "a/1dE1T4oBgHgl3EQf5AXg/content/tmp_files/load_file.txt" "b/1dE1T4oBgHgl3EQf5AXg/content/tmp_files/load_file.txt" new file mode 100644--- /dev/null +++ "b/1dE1T4oBgHgl3EQf5AXg/content/tmp_files/load_file.txt" @@ -0,0 +1,1509 @@ +filepath=/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf,len=1508 +page_content='1 Nonlinear THz Control of the Lead Halide Perovskite Lattice Maximilian Frenzel1,*, Marie Cherasse1,2,*, Joanna M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Urban1, Feifan Wang3,‡ , Bo Xiang3, Leona Nest1, Lucas Huber3,§, Luca Perfetti2, Martin Wolf1, Tobias Kampfrath1,4, X.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='-Y.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Zhu3, Sebastian F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Maehrlein1,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='† 1 Fritz Haber Institute of the Max Planck Society,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Department of Physical Chemistry,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Berlin,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Germany 2 LSI,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' CEA/DRF/IRAMIS,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' CNRS,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Ecole Polytechnique,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Institut Polytechnique de Paris,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Palaiseau,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' France 3 Columbia University,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Department of Chemistry,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' New York City,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' USA 4 Freie Universität Berlin,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Berlin,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Germany Authors contributed equally ‡ Present address: Department of Materials,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' ETH Zurich,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 8093 Zürich,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Switzerland § Present address: Sensirion AG,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Staefa,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Switzerland † Corresponding author.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Email: maehrlein@fhi.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='mpg.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='de Abstract Lead halide perovskites (LHPs) have emerged as an excellent class of semiconductors for next-generation solar cells and optoelectronic devices.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Tailoring physical properties by fine-tuning the lattice structures has been explored in these materials by chemical composition or morphology.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Nevertheless, its dynamic counterpart, phonon-driven ultrafast material control, as contemporarily harnessed for oxide perovskites, has not been established yet.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Here we employ intense THz electric fields to obtain direct lattice control via nonlinear excitation of coherent octahedral twist modes in hybrid CH3NH3PbBr3 and all-inorganic CsPbBr3 perovskites.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' These Raman-active phonons at 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='9 – 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 THz are found to govern the ultrafast THz-induced Kerr effect in the low- temperature orthorhombic phase and thus dominate the phonon-modulated polarizability with potential implications for dynamic charge carrier screening beyond the Fröhlich polaron.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Our work opens the door to selective control of LHP’s vibrational degrees of freedom governing phase transitions and dynamic disorder.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Introduction During the last decade, lead halide perovskites (LHPs) emerged as promising semiconductors for efficient solar cells, light-emitting diodes, and other optoelectronic devices (1-3).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Key prerequisites for the high LHP device efficiencies are the long charge carrier diffusion lengths and lifetimes (4, 5), often explained by the unusual defect physics (6, 7) and/or dynamic charge carrier screening (8, 9).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The latter relies on delicate electron-phonon coupling, established by the dominant role of the static structure and dynamics of the lead-halide framework (10, 11).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' However, the exact mechanisms of the carrier-lattice interaction in the highly polarizable and anharmonic LHP lattices remain debated (12, 13).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The sensitivity of the physical properties to structural distortions is a common feature in the extensive family of perovskites.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In particular, for oxide perovskites, the control of specific lattice modes leads to ultrafast material control and nonlinear phononics (14, 15).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Successful examples include, among others, light-induced superconductivity (16), magnetization switching (17), access to hidden quasi-equilibrium spin states (18), ferroelectricity (19, 20) and insulator-metal transitions (21) in perovskite or similar garnet structures.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The crystal structure of LHPs features a large A-site cation surrounded by PbX6 octahedra consisting of lead (Pb) and halide (X) ions in the ABX3 crystal structure (see Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1A).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The 2 electronic band structure is mainly determined by the identities of metal and halide but is also highly sensitive to the Pb-X-Pb bond angle, which can be controlled through the steric hindrance of the A-cation (22).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Changing the Pb-X-Pb bond angle is equivalent to tilting of the PbX6octahedra, which serves as an order parameter for the cubic \uf0e0 tetragonal \uf0e0 orthorhombic phase transitions (23, 24).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Octahedral tilting is also an important factor governing structural stability (25), dynamic disorder (26, 27), and potential ferroelectricity (26, 27) in LHPs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A recent study using resonant excitation of the ~1 THz octahedral twist mode (Pb-I-Pb bending) revealed modulation of the bandgap of CH3NH3PbI3 at room temperature (28).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A similar observation of dynamic bandgap modulation due twist modes was made at 80K for off-resonant impulsive Raman excitation (29).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' These twist modes are also believed to contribute to the formation of a polaronic state (30).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' All of these findings indicate an intriguing role of carrier coupling to Raman-active non-polar phonons in addition to the polar LO phonons in the conventional Fröhlich polaron picture (11, 31).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In addition, the application of the Fröhlich polaron picture to LHPs has been questioned (9, 26), because of the limited applicability of the harmonic approximation in these soft lattices (13).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Accordingly, the dynamic screening picture in LHPs is incomplete and its microscopic mechanism continues to be debated (32, 33).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Furthermore, identifying and characterizing polaronic behavior is experimentally difficult (31, 33-37).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Optical Kerr effect (OKE) in LHPs (38, 39) did not succeed in unveiling a lattice response and can be explained by an instantaneous electronic polarization (due to hyperpolarizability) instead (40).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Moreover, previous strong field THz excitation could not directly detect the driven vibrational modes (28, 31) and coherent control of the phonons remained elusive.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Here, we turn to the THz-induced Kerr effect (TKE) (41, 42) to investigate lattice-modulated polarization dynamics in the electronic ground state.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We employ intense THz electric fields (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1B) that broadly cover most of the inorganic cage modes (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1C) and may nonlinearly probe the THz polarizability.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The rapidly changing single-cycle THz field macroscopically mimics the sub-picosecond variation of local electric fields following electron-hole separation (43, 44) and elucidates the isolated lattice response.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Experiment Generally, the polarizability describes the tendency of matter to form an electric dipole moment when subject to an electric field, such as the local field from a mobile charge carrier in a semiconductor.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In the presence of an electric field 𝑬, the microscopic dipole moment is given by 𝒑(𝑬) = 𝝁0 + 𝛼𝑬, where 𝜇0 is the static dipole moment and 𝛼 is the polarizability tensor.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In LHPs 𝛼 originates from three contributions: instantaneous electronic response (𝛼e), lattice distortion (𝛼lat), and molecular A cation reorientation (𝛼mol).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For small perturbations of the respective collective coordinate 𝑄 (charge distribution, molecular orientation, or lattice mode) a Taylor expansion yields 𝒑(𝑬, 𝑄) = 𝝁0 + 𝜕𝝁𝟎 𝜕𝑄 𝑄 + 𝜕𝛼 𝜕𝑄 𝑄𝑬 , (1) where the two partial derivatives correspond to the mode effective charge 𝑍∗ and the Raman 𝑅𝑖𝑗 tensor, respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Macroscopically, the two terms lead to lattice polarization 𝑍∗𝑄IR and phonon-modulated susceptibility 𝜒eq (1) + (𝜕𝜒eq (1)/𝜕𝑄R)𝑄R for polar, 𝑄IR, and non-polar, 𝑄R, modes, respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The latter relates 𝜕𝛼/𝜕𝑄 to a transient dielectric function and change in refractive index of the material.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This relation thus enables studying microscopic polarizability through the observation of macroscopic transient birefringence induced by a pump pulse and experienced by a weak probe pulse (41, 45).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Collective polarization dynamics are induced by the driving force 𝐹 = −𝜕𝑊int/𝜕𝑄, where 𝑊int = −𝑷(𝑬, 𝑄) ∙ 𝑬 is the potential energy of the macroscopic polarization 𝑷 = ∑ 𝒑𝑖 𝑖 interacting with an electric field 𝑬 (from a local charge 3 carrier or through light-matter coupling in the electric dipole approximation).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Thus, two 𝐸THz interactions lead to THz polarizability-induced transient birefringence in TKE (42), which is linearly probed by a weak probe pulse 𝐸pr in an effective 3rd order nonlinear process proportional to 𝜒(3)𝐸THz𝐸THz𝐸pr (see Methods) (41, 46).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' To induce polarization dynamics, we use intense THz single-cycle pulses with a 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 THz center frequency (> 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 THz spectral width, see Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1C), delivering sub-picosecond peak electric fields exceeding 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 MV/cm generated by optical rectification in LiNbO3 (47).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We probe the resulting transient birefringence, i.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='e.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' anisotropic four-wave mixing signals, by stroboscopic sampling with a synchronized 20 fs pulse (800 nm center wavelength) in a balanced detection scheme, see Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1A.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We therefore effectively measure a 3rd order nonlinear signal field heterodyned with the transmitted probe field.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The probe pulses are linearly polarized at 45° with respect to the vertically polarized THz pulses.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' As representative LHPs, we investigate hybrid organic-inorganic CH3NH3PbBr3 (MAPbBr3) and fully inorganic CsPbBr3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The freestanding single crystal samples (200 – 500 µm thickness) were solution grown by an antisolvent diffusion method (48, 49) (see Methods).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Complementary polycrystalline thin films (~ 400 nm thickness) were spin-coated on 500 µm BK7 substrates, being particularly technologically relevant as most state-of-the-art LHP solar cells are fabricated in a similar way (50).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Results Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2A shows the THz induced transient birefringence in MAPbBr3 single crystals at room temperature.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The signal (blue line) initially follows 𝐸THz 2 (grey area, measured via electrooptic sampling), but then transitions into a nearly mono-exponential decay for time delays 𝑡 > 500 fs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The transient birefringence peak at 𝑡 = 0 clearly scales quadratically with the THz-field amplitude as found by the pump fluence dependence in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2B.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' With the exponential decay dynamics remaining also constant for different fluences (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S2), we can infer the Kerr-type origin of the full signal and thus conclude a strong THz polarizability.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Furthermore, the peak amplitude’s (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2C) and the exponential tail’s (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S3) dependence on the azimuthal angle between probe polarization direction and crystal axes perfectly obeys the expected 4-fold rotational symmetry of the 𝜒(3) tensor and TKE dependence of 𝜒𝑖𝑗𝑘𝑙 (3) 𝐸𝑗 THz𝐸𝑘 THz𝐸𝑙 pr.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We quantify the THz polarizability of MAPbBr3 by a nonlinear THz refractive index 𝑛2 of about 2 × 10−14 cm2/W (see details in SI), being on the same order as in the optical region (51) and roughly 80 times larger than 𝑛2 of Diamond (52), which is known as a suitable material for THz nonlinear optics (53).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The small oscillatory deviations from the exponential tail in MAPbBr3 (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2A), become more pronounced and qualitatively different in CsPbBr3 in the form of a bumpy, non-trivial shape (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2D).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This stark difference between MAPbBr3 and CsPbBr3 is reminiscent of 2D-OKE results (40), where the oscillatory signal of CsPbBr3 was found to be mainly due to anisotropic light propagation, since CsPbBr3 is orthorhombic and thus birefringent at room temperature.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The fluence (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2E) and azimuthal dependences (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2F) are consistent with the pure 3rd order nonlinearity of the signal.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' However, fits to the azimuthal angle dependences in Figs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2C,F (black lines) yield different ratios of the off-diagonal 𝜒𝑖𝑗𝑘𝑙 (3) to diagonal 𝜒𝑖𝑖𝑖𝑖 (3) tensor elements for the two materials: 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 for MAPbBr3 and 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 for CsPbBr3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A similar polarization dependence of static Raman spectra was recently attributed to additional isotropic disorder from the rotational freedom of the polar MA+ cation in MAPbBr3 (54).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 4 Figs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 3A,B show a comparison of the temperature dependent TKE in MAPbBr3 single crystals and polycrystalline thin films.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' At room temperature (both top traces), it stands out that the thin film TKE signal lacks the exponential decay seen in the single crystals, providing a first evidence that the tail stems from dispersion effects and is not due to intrinsic molecular relaxation dynamics as previously interpreted (55).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A strong and sophisticated THz dispersion, as seen in Fig 1C, is a general, but often overlooked, phenomenon in broadband high-field THz pump-probe spectroscopy.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In analogy to the OKE (40), the features of the room temperature TKE in both MAPbBr3 and CsPbBr3 might therefore be dominated by dispersive and anisotropic light propagation.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Hence, we assign the main contribution of the TKE response at room temperature to the instantaneous electronic polarizability (hyperpolarizability), which may overwhelm possible lattice contributions.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This interpretation will be further supported by the modeling below.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' From here on, we mainly focus on the TKE of MAPbBr3, especially at low temperatures at which increased phonon lifetimes should facilitate the observation of a coherent lattice response (54, 56).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For the single crystal (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 3A), the TKE dynamics at 180 K are different than at room temperature, which might reflect the change of structural phase from cubic to tetragonal.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' At 180K, an oscillatory signal at short times (< 2 ps) appears, suggesting the presence of a coherent phonon which was overdamped in the cubic phase at room temperature (54).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The coherent oscillations become much stronger for the single crystal at 80 K, where MAPbBr3 is in the orthorhombic phase.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Less pronounced, but clear oscillations are also visible in the thin film sample at 80 K (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 3A, lowest trace).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We extract the oscillatory parts, Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 3C, of both single crystal and thin film samples at 80 K by subtracting incoherent backgrounds, using a convolution of the squared THz field with a bi-exponential function.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The respective Fourier transforms in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 3D reveal the same oscillations frequency of 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='15 ± 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='05 THz for both samples.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This clearly rules out anisotropic propagation effects as the origin of these oscillations (40), as the 400 nm film is too thin for significant walk-off between pump and probe (shown in simulations later) and the different thicknesses of the two samples rule out a Fabry-Pérot resonance effect.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Thus, we can clearly assign the signal to a lattice-modulation of the THz polarizability dominated by a single 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='15 THz phonon in MAPbBr3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We now turn to THz-THz- VIS four-wave-mixing simulations to understand the origins of TKE from MAPbBr3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Modelling For dispersive and birefringent materials, the Kerr signal cannot be decomposed into an effective birefringence change observed by an independent probe beam (46).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Instead, the Kerr- effect induced nonlinear polarization 𝑃(3) needs to be captured in a full four-wave-mixing (FWM) picture.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' To separate the three polarizability contributions (instantaneous electronic,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' molecular and lattice) and to take anisotropic light propagation across dispersive phonon resonances into account,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' we simulate the 3rd order nonlinear polarization by 𝑃𝑖 (3)(𝑡,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 𝑧) = 𝜖0 � 𝑑𝑡′ � 𝑑𝑡′′ 𝑡′ −∞ � 𝑑𝑡′′′ 𝑡′′ −∞ 𝑡 −∞ 𝑅�𝑖𝑗𝑘𝑙𝑅(𝑡,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 𝑡′,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 𝑡′′,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 𝑡′′′)𝐸𝑗 THz(𝑡′,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 𝑧)𝐸𝑘 THz(𝑡′′,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 𝑧)𝐸𝑙 pr(𝑡′′′,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 𝑧),' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (2) where 𝑅 is the time-domain 𝜒(3) response function (46) and 𝐸THz and 𝐸pr are the pump and probe electric fields,' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The time-independent 𝑅�𝑖𝑗𝑘𝑙 tensor constitutes the respective 𝜒(3) symmetry for the different crystalline phases, in agreement with the ratios of the tensor elements obtained from the azimuthal fits in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2C.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For the instantaneous electronic polarizability (hyperpolarizability), we assume temporal Dirac delta functions 𝑅e(𝑡, 𝑡′, 𝑡′′, 𝑡′′′) = 𝑅e,0𝛿(𝑡 − 𝑡′)𝛿(𝑡′ − 𝑡′′)𝛿(𝑡′′ − 𝑡′′′).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For a lattice response, we model the driven phonon response by a Lorentz oscillator 5 𝑅ph(𝑡, 𝑡′, 𝑡′′, 𝑡′′′) = 𝑅ph,0𝛿(𝑡′ − 𝑡′′)𝛿(𝑡′′ − 𝑡′′′)𝑒−Γ�𝑡−𝑡′� sin ���𝜔ph 2 − Γ2�(𝑡 − 𝑡′)�, (3) where 𝜔ph/2𝜋 is the frequency and 1/2Γ the lifetime of the phonon (46).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The driving force for Raman-active phonons is hereby 𝐸𝑗 THz𝐸𝑘 THz, which contains difference- and sum-frequency terms (57, 58).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The latter is a unique distinction to the OKE.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For 𝐸THz we can directly use the experimental THz electric field, as measured in amplitude and phase resolved electro-optic sampling.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' After we determine the complex refractive indices (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1C) and extrapolate the static birefringence (see Methods and SI), we calculate and propagate all involved fields from Eq.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (2) incl.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' signal fields 𝐸𝑖 s(𝑡, 𝑧) emitted from 𝑃𝑖 (3)(𝑡, 𝑧), followed by our full detection scheme, including balanced detection, to obtain the pump-probe signal (see details in Methods).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 4A shows the simulated TKE signal (grey) compared to the experimental data (blue) at room temperature for a 500 µm thick MAPbBr3 single crystal.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' It unveils the formation of a long exponential tail produced by walk-off, dispersion, and absorption effects, even for only an instantaneous electronic response 𝑅e.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This confirms that the electronic polarizability dominates the TKE signal at room temperature.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' It contrasts a previous interpretation of a TKE measurement in thick single crystal MAPbBr3, which neglected propagation effects entirely (55).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' At 80 K, MAPbBr3 is orthorhombic.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We therefore need to include additional static birefringence.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Instantaneous hyperpolarizability alongside static birefringence and dispersion can cause the appearance of oscillatory features (40).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Nevertheless, our modelling finds these features to be too short-lived (see Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S14) to explain our experimental observation at 80 K.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Thus, we need to account for both hyperpolarizability 𝑅e and lattice-modulated polarizability 𝑅ph responses (fit parameters: 𝜔ph/2𝜋 = 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='14 THz, Γ = (2 ∙ 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='7ps)−1, 𝑅e,0/𝑅ph,0 = 2.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4) to describe the low-temperature TKE signals in the time- and frequency domain (Figs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 4B,C).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In contrast to OKE at 80K (40), the oscillations in TKE are therefore due to coherent phonon modes and we hence finally observe an ultrafast lattice response to a sub-picosecond electric field transient.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The simulation assuming only instantaneous hyperpolarizability for a 400 nm thin film agrees well with the experimental TKE at room temperature (see Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 4D).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' As expected, the simulation lacks the clear tail seen in the thick single crystals, thereby additionally confirming that the tail is due to light propagation effects.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Also here, at 80 K, we need to include both instantaneous electronic and phonon contributions (𝜔ph/2𝜋 = 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='14 THz, Γ = (2 ∙ 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='7ps)−1, 𝑅e,0/𝑅ph,0 = 24) to describe the experimental signals for the thin films in Figs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 4E,F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Here, a purely instantaneous electronic contribution alongside static birefringence does not lead to oscillatory features (see Figs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S14A,C).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This provides direct proof that the observed oscillations in Figs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 3C,D originate from a coherent phonon.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Therefore, through comparison of single crystals with thin films and by rigorous FWM simulation, we prove to witness a coherent lattice-driven dynamic polarization response.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Interpretation Besides potential rotational disorder, our rigorous modeling shows that we do not observe a TKE contribution that we can unambiguously relate to an ultrafast cation reorientation in the form of a liquid-like exponential decay (41, 42).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We rather find MAPbBr3‘s TKE tail at room temperature to be most likely overwhelmed by the instantaneous hyperpolarizability 𝑅e in conjunction with dispersive light propagation.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This might be also explained by the THz pump spectrum being far off the cation rotational resonances around the 100 GHz frequency range (59).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The cation species nevertheless influences the static and dynamic properties of the inorganic lattice, highlighting the importance of the interplay between the organic and inorganic 6 sub-lattices for the LHPs equilibrium structure (56).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This fact shows up e.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='g.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' as a single dominating PbBr6 cage mode in MAPbBr3 but two dominating modes in CsPbBr3 (see Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S1);' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' in agreement with static Raman spectra (54).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The various templating mechanisms by which the cation influences these properties (60) are through its steric size (22), lone-pair effects (27, 61), or hydrogen bonding (62).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For MAPbBr3, we find a single phonon mode dominating the Raman-active lattice dynamics in response to a sub-ps electric field spike.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The observed phonon at 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='15 THz is consistent with static Raman spectra in the visible range, where this mode also exhibits the highest scattering amplitude (54, 63).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Thus, we can assign it to a dynamic change in the Pb-Br-Pb bond angle corresponding to a twisting of the PbBr6 octahedra (twist mode) (64).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Based on theory work for MAPbI3 (65), we assign this to Ag symmetry, which matches the experimental observations that the mode is still present when we rotate the single crystal by 45° (see Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S7) and that we also observe the same mode in polycrystalline thin films (Figs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 3C,D).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We suggest that at room temperature this mode also strongly modulates the THz dielectric response, even though its oscillations are potentially overdamped as inferred from the broad Raman spectra (54, 56).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' To distinguish whether this twist mode only dominates the ultrafast lattice response in MAPbBr3, or is of wider relevance for other LHPs, we analyze the TKE response of CsPbBr3, where we observe two modes at 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='9 and 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 THz at 80K (see Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S1), corresponding to two octahedra twist modes as observed in static Raman spectra (54).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We thus conclude that the transient THz polarizability (𝜕𝜒eq (1)/𝜕𝑄) 𝑄 is generally dominated by the octahedra twist modes in LHPs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We now consider the excitation mechanism of the coherent phonon.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 5A shows that the 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='15 THz oscillations at 80K scale with the square of the THz electric field amplitude, suggesting nonlinear excitation with a Raman-type driving force.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This is consistent with the Kerr effect being also a Raman-type probing mechanism.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Generally, there are four types of Raman-active THz excitation mechanisms: Difference- or sum-frequency excitation via Ionic Raman Scattering (IRS) or Stimulated Raman Scattering, corresponding to nonlinear ionic (=phononic) or nonlinear electronic (= photonic) pathways, respectively (58).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Indeed, the Ag symmetry of the observed modes permits IRS, where a resonantly driven IR-active phonon couples anharmonically to a Raman-active mode (14, 58).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' However, this phononic pathway requires phonon anharmonicity, whereas the photonic pathway requires electronic THz polarizability.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The sum-frequency (SF) and difference-frequency (DF) photonic force spectra in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 5B indicate a comparable probability for both photonic mechanisms to drive the 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='15 THz mode (dashed line).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For the phononic pathways in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 5C, the DF excitation requires a primarily driven IR-active phonon with a bandwidth of ≳ 1 THz, which exists in our excitation range even at 80 K (66).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' On the other hand, there are also IR-active modes, which provide roughly half the frequency of the Raman-active mode ΩIR = ΩR/2 enabling phononic SF-IRS (58).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Accordingly, none of the four nonlinear excitation pathways can be neglected, but the observed strong electronic THz polarizability in conjunction with a longer penetration depth for lower THz frequencies favors a SF nonlinear photonic mechanism.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We leave the determination of the exact excitation pathway to further studies, e.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='g.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' by two-dimensional TKE (67) or more narrowband THz excitation (68).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Discussion Independent of the precise excitation pathway and in contrast to optical Raman or transient absorption studies, we unambiguously observe strong electron-phonon coupling of the octahedral twist modes via a pure THz polarizability (electronic or ionic).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This explains the mode’s dominating influence on the electronic bandgap in MAPbI3 previously observed by Kim et al.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (28).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The twist mode’s half-cycle period of ~0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 ps is short enough to contribute to 7 electron-phonon coupling within the estimated polaron formation time (69), even in the overdamped case at room temperature.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We can understand carrier screening by non-polar modes as follows.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' As shown in Eq.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (1), the THz polarizability contains two lattice contributions: From polar lattice modes 𝑃IR(𝜔) ∝ 𝑍∗𝑄IR(𝜔) ∝ 𝑍∗𝐸THz(𝜔) and from the non- resonant electron cloud moving at THz speeds (sub-ps time scales): 𝑃𝑒(𝜔) = 𝜖0[ 𝜒𝑒 (1)(𝜔) + 𝜕𝜒𝑒 (1) 𝜕𝑄R (𝜔, 𝛺) 𝑄R(𝛺) ]𝐸THz(𝜔), (4) where the latter is modulated in the presence of a Raman-active phonon 𝑄R.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Thus, excited Raman-active modes lead to a transient dielectric response 𝜖(ω) = 𝜖𝑒𝑞(ω) + Δ𝜖(𝜔, Ω) at THz frequencies 𝜔 with Δ𝜖 = 𝜕𝜒𝑒 (1) 𝜕𝑄R 𝑄R, which constitutes an additional contribution of higher order screening due to a fluctuating lattice.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In the macroscopic incoherent case, Δ𝜖 averages out.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' On time and length scales relevant to electron-hole separation and localization (< 1 nm and < 1ps) (43, 44), collective octahedral tilting produces (70) an additional THz polarizability, which might add to the conventional Fröhlich picture of carrier screening.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We speculate that a local non-zero twist angle 𝑄R could be either already present due to dynamic disorder (see discussion below), or might be nonlinearly excited by the transient local charge field 𝐸loc 2 , easily exceeding 1 MV/cm (9) (analog to the excitation pathways above).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The latter scenario agrees with MAPbBr3’s unusually large optical 𝜒(3), previously attributed to local confinement effects (51).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The observed 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='15 THz mode is therefore a good candidate for contributing to strong electron- phonon coupling beyond the polar Fröhlich picture.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The driven twist mode is similar to soft modes in oxide perovskites, where the tilting angle of adjacent oxygen octahedra is an order parameter for phase transitions (71).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Recently, TKE was similarly employed to drive and detect ultrafast field-induced ferroelectricity in the quantum paramagnet SrTiO3 (19).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In Eu and Sr doped La2CuO4, driving the tilt of oxygen octahedra was found to induce signatures of superconductivity persisting over a few ps above the critical temperature (16).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Consistent with these observations in oxide perovskites, the tilting angle of the PbX6 octahedra (twist mode) was found to act as an order parameter for phase transitions in LHPs (23, 24) and in the double-perovskite Cs2AgBiBr6 (72).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Especially for MAPbBr3, the Raman scattering intensity of the 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 THz peak was recently shown as measure of the orthorhombic-tetragonal phase transition (63) and its spectral evolution in Raman (56) and neutron scattering (73) is indicative of a soft mode phase transition.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Yet, the LHP lattice properties were previously mainly tuned in a static and chemical manner, e.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='g.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' by acting on the octahedral tilting angle through the steric size of the A-site cation (22).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The coherent lattice control demonstrated here allows dynamic tuning of the structure and thus ultrafast phonon- driven steering of LHP’s optoelectronic properties, e.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='g.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' for integrated photonic devices operating at GHz to THz clock-rates (74).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In addition, imposing a coherence on the octahedral tilting should directly influence the dynamic disorder (75), which is considered one of the key components determining the optoelectronic properties of LHPs (12, 54, 76).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Dynamic disorder means that the effective crystallographic structure (e.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='g.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' cubic at 300 K) only exist in spatial and temporal average.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Specifically, in LHPs with a Goldschmidt tolerance factor below 1, such as MAPbBr3 and CsPbBr3, the disorder mainly arises from the lattice instability associated with octahedral tilting (61, 75, 77), evidenced by X-ray total scattering in CsPbBr3 (78), inelastic X-ray scattering in MAPbI3 (70) and Raman spectroscopy in MAPbBr3, CsPbBr3 and MAPbI3 (54, 77).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The resulting fluctuating lattice potential and polar nanodomains have been suggested as underlying mechanisms for dynamic charge carrier screening in the form of preferred current pathways 8 (79, 80) and ferroelectric polarons (26, 81), respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' All these phenomena might be potentially controlled or temporally lifted by the THz control of octahedral motion.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Overall, we find that the octahedral tilting motion, which serves as an order parameter for phase transitions (23, 24) and contributes significantly to dynamic disorder (54, 77), shows a strong nonlinear coupling to a rapidly varying electric field on sub ps-timescales that are relevant to local electron-hole separation polaron formation.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Our results thus indicate that the TO octahedral twist mode contributes to strong electron-phonon coupling and dynamic carrier screening in LHPs, which may be inherently linked to a local and transient phase instability as suggested by the ferroelectric polaron picture (26, 81).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Conclusion By investigating 3rd order nonlinear polarization dynamics in hybrid and all-inorganic LHPs, we reveal that the room temperature TKE response stems predominantly from a strong THz hyperpolarizability, leading to a nonlinear THz refractive index on the order of 10-14 cm2/W.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In analogy to previous OKE studies (40), we explain and model the appearance of retarded TKE dynamics by dispersion, absorption, walk-off, and anisotropy effects (46).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' These effects are of crucial relevance to contemporary THz pump-probe experiments, such as TKE or THz-MOKE studies (82, 83).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For sufficiently long phonon lifetimes at lower temperatures, we can nonlinearly drive and observe a coherent lattice response of the ~1 THz octahedral twist mode(s).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' These phonons couple most strongly to the THz polarizability, which means they must be highly susceptible to transient local fields on the 100s fs time scale, relevant to electron- phonon coupling and carrier localization.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We find this ultrafast non-polar lattice response to be mediated by anharmonic phonon-phonon coupling and/or by the strong nonlinear electronic THz polarizability.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The same octahedral twist mode serving as a sensitive order parameter for structural phase transitions (63, 73) is likely the origin of significant intrinsic dynamic disorder in LHPs (54, 75).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Thus, our findings suggest that the microscopic mechanism of the unique defect tolerance (39, 84) and long carrier diffusion lengths (4, 5) of LHPs might also rely on small phase instabilities accompanying the polaronic effects.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Our work demonstrates the possibility of coherent control over the twist modes via nonlinear THz excitation.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Since the octahedral twist modes are the dynamic counterparts to steric engineering of the metal-halide-metal bond angle, our work paves the way to study charge carriers in defined modulated lattice potentials, to control dynamic lattice disorder, or to macroscopically switch polar nanodomains leading to the emergence of transient ferroelectricity.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 9 Materials and Methods Sample Growth The single crystal samples were synthesized based on our previous published method (40).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For MAPbBr3, the precursor solution (0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='45 M) was prepared by dissolving equal molar ratio of MABr (Dyesol, 98%) and PbBr2 (Aldrich, ≥98%) in dimethylformamide (DMF, Aldrich, anhydrous 99.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8%).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' After filtration, the crystal was allowed to grow using a mixture of dichloromethane (Aldrich, ≥99.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5%) and nitromethane (Aldrich, ≥96%) as the antisolvent (48).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Similar method was used for CsPbBr3 crystal growth (49).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The precursor solution (0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='38 M) was formed by dissolving equal molar ratio of CsBr (Aldrich, 99.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='999%) and PbBr2 in dimethyl sulfoxide (EMD Millipore Co.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', anhydrous ≥99.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8%).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The solution was titrated by methanol till yellow precipitates show up and did not redissolve after stirring at 50 °C for a few hours.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The yellow supernatant was filtered and used for the antisolvent growth.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Methanol was used for the slow vapor diffusion.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' All solid reactants were dehydrated in a vacuum oven at 150 °C overnight and all solvents were used without further purification.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Thin films.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Before spin-coating, the substrate was rinsed by acetone, methanol and isopropanol and treated under oxygen plasma for 10 min.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The freshly prepared substrate was transferred to the spin coater within a short time.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For MAPbBr3, the precursor DMSO (Aldrich, ≥99.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='9%) solution (2M) containing the equimolar ratio of MABr and PbBr2 was used for the one-step coating method.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The film was formed by spin-coating at 2000 rpm for 45 s and annealed at 110 °C for 10 min.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For CsPbBr3, a two-step method was implemented.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' First, the PbBr2 layer was obtained by spin-coating the 1 M PbBr2/DMF precursor solution at 2000 rpm for 45 s and dried at 80 °C for 30 min.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Subsequently, the PbBr2 film was immersed in a 70 mM CsBr/methanol solution for 20 min.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Following the rinsing by isopropanol, the film was annealed at 250 °C for 5 min to form the uniform perovskite phase.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' THz-induced Kerr effect THz pulses with 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 THz center frequency and field strength exceeding 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 MV/cm (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1B,C), were generated by optical rectification in LiNbO3 with the tilted pulse front technique (47).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' To that end, LiNbO3 was driven by laser pulses from an amplified Ti:sapphire laser system (central wavelength 800 nm, pulse duration 35 fs FWHM, pulse energy 5 mJ, repetition rate 1 kHz).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The probe pulses came from a synchronized Ti:sapphire oscillator (center wavelength 800nm, repetition rate 80 MHz) and were collinearly aligned and temporarily delayed with respect to the THz pulse.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The probe polarization was set at 45 degrees with respect to the vertically- polarized THz pulses.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The THz pulses induced a change in birefringence (TKE) in the sample (41).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This birefringence causes the probe field to acquire a phase difference between polarization components parallel and perpendicular to THz pulse polarization.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The phase difference is detected via a half- and quarter-waveplate (HWP and QWP) followed by a Wollaston prism to spatially separate perpendicularly polarized probe beam components.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The intensity of the two beams is detected by two photodiodes in a balanced detection configuration.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Four-wave-mixing simulation The 3rd order nonlinear polarization 𝑃(3)(𝑡, 𝑧) is simulated using the general four-wave mixing equation (Eq.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (2)) and according to Ref.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (46).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' To compute 𝑃(3)(𝑡, 𝑧), all three contributing light fields, 𝐸𝑗 THz, 𝐸𝑘 THz and 𝐸𝑙 pr, are propagated through the crystal on a time-space grid.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The three fields inside the sample are calculated at any location 𝑧 using 𝐸𝑖(𝑡, 𝑧) = � 𝑡𝑖(𝜔)𝐴𝑖(𝜔)𝑒−𝑖(𝜔𝑡−𝑘𝑖(𝜔)𝑧)(1 − 𝑅𝑖(𝜔, 𝑧))𝑑𝜔 ∞ −∞ , (5) with 10 𝑅𝑖(𝜔, 𝑧) = 𝑟𝑖�1 + 𝑒2𝑖𝑧𝑘𝑖(𝜔)� 𝑒2𝑖(𝑑−𝑧)𝑘𝑖(𝜔) 1 − 𝑟𝑖 2(𝜔)𝑒2𝑖𝑑𝑘𝑖(𝜔) , (6) where 𝐴𝑖(𝜔) is the spectral amplitude of the field and 𝑡𝑖 and 𝑟𝑖 denote the Fresnel transmission and reflection coefficients respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' As the input pump field 𝐸THz we use the full experimental THz electric field generated via optical rectification in LiNbO3 as measured using electro-optic sampling in Quartz (85).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For the probe field 𝐸pr we assume a Fourier limited Gaussian spectrum with center wavelength 800 nm and pulse duration 20 fs, experimentally measured by a spectrometer and a commercial SPIDER.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For both non-birefringent and birefringent simulations, we use the THz refractive index for MAPbBr3 as calculated from its dielectric function based on the experimental work by Sendner et al.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (10) (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S11).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In the optical region, the precise anisotropic refractive index of CsPbBr3 is used as measured using the 2D-OKE (46).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For the birefringent lead halide perovskite simulation, the static birefringence of CsPbBr3 is used and interpolated to THz region (Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S12).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For the isotropic cubic perovskite, the static birefringence is set to zero.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In the shown simulation results, the time-grid had a finite element size of Δ𝑡′ = 16.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 fs and the spatial grid had a finite element size of Δ𝑧 = 10 μm for the single crystal and Δ𝑧 = 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 μm for the thin film simulations respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' These values were chosen for the sake of computational efficiency and did not qualitatively affect the simulation results.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The pump-probe delay finite element size was chosen to be Δ𝑡 = 16.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 fs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' We assume that the nonlinear polarization 𝑃(3) emits an electric field 𝐸(4) at every slice 𝑧 according to the inhomogeneous wave equation [∇2 + 𝑘𝑖 2(𝜔)]𝐸𝑖 (4)(𝜔, 𝑡, 𝑧) = − 𝜔2 𝜖0𝑐2 𝑃𝑖 (3)(𝜔, 𝑡, 𝑧), (7) which then co-propagates with the probe field 𝐸pr.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The transmitted probe field 𝐸pr and emitted field 𝐸(4) are projected on two orthogonal polarization components by propagating through a half-wave plate, quarter-wave plate and Wollaston prism.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The combined effect of these optical devices are captured by the Jones matrices 𝐽1 and 𝐽2 for the two separated polarization component channels.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A balanced detection scheme allows observation of 𝐸(4) by interfering with 𝐸pr.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Under balanced conditions, the detected non-equilibrium signal is 𝑆 ∝ ∫ 𝑅𝑒�(𝐽1𝐸𝑝𝑟) ∙ �𝐽1𝐸(4)∗� − (𝐽2𝐸𝑝𝑟) ∙ �𝐽2𝐸(4)∗��𝑑𝜔.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (8) Our simulation therefore mimics the balancing conditions of the experiment.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A detailed description of this calculation is given in (46).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' To model the response of the system, we assume the response function 𝑅e(𝑡, 𝑡′, 𝑡′′, 𝑡′′′) for an instantaneous electronic response and 𝑅ph(𝑡, 𝑡′, 𝑡′′, 𝑡′′′) for a phonon response.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The expressions for 𝑅e and 𝑅lat are given in the main paper.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In the frequency domain, 𝑅(𝜔) = 𝜒(3)(𝜔).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For normal incidence on the (101) crystal surface, the orthorhombic space group Pnma allows Kerr signals from 𝜒𝑥𝑥𝑥𝑥 (3) , 𝜒𝑦𝑦𝑦𝑦 (3) , 𝜒𝑥𝑥𝑦𝑦 (3) = 𝜒𝑥𝑦𝑦𝑥 3 = 𝜒𝑥𝑦𝑥𝑦 (3) and 𝜒𝑦𝑦𝑥𝑥 (3) = 𝜒𝑦𝑥𝑥𝑦 (3) = 𝜒𝑦𝑥𝑦𝑥 (3) (40).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' While the cubic space group Pm3m and allows for 𝜒𝑥𝑥𝑥𝑥 (3) = 𝜒𝑦𝑦𝑦𝑦 (3) and 𝜒𝑥𝑥𝑦𝑦 (3) = 𝜒𝑥𝑦𝑦𝑥 (3) = 𝜒𝑥𝑦𝑥𝑦 (3) = 𝜒𝑦𝑦𝑥𝑥 (3) = 𝜒𝑦𝑥𝑥𝑦 (3) = 𝜒𝑦𝑥𝑦𝑥 (3) .' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The Pnma space group applies to CsPbBr3 in its orthorhombic phase, which is the case for all temperatures considered in this work.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The Pm3m space applies to MAPbBr3 for its room temperature cubic phase.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' All allowed tensor elements were assumed to have the same magnitude.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Simulations for an electronic response only and without optical anisotropy are shown for various thicknesses in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S13.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This applies to MAPbBr3 single crystals at room temperature when this material is in the cubic phase.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Simulations for an electronic response only and with optical anisotropy are shown for various thicknesses in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S14.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This applies to MAPbBr3 in its low-temperature orthorhombic phase and CsPbBr3, which is orthorhombic for all temperatures considered in this work.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The effect of optical anisotropy on the TKE is very 11 dependent on the azimuthal angle of the crystal.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Results are shown for two different azimuthal angles: 0° and 45° angle between crystal axis and probe polarization in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S14.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S14 shows that the oscillatory features due to propagation effects and static birefringence cannot explain the oscillations observed in low temperature MAPbBr3 single crystals and thin films.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' To simulate this oscillatory signal, we have to consider both electronic and phonon contributions to 𝑅 = 𝑅e + 𝑅ph alongside static birefringence.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The chosen simulation parameters are given in the main text and were chosen in accordance with the Lorentzian fits to our experimental data in 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metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Wolf, S.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Kovalev, M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Sajadi, Optical Rectification and Electro-Optic Sampling in Quartz.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' ArXiv, (2022).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 15 Figures Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1 | THz fields for nonlinear lattice control in lead halide perovskites.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Sketch of the experimental pump-probe configuration.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' An intense THz electric field causes a transient change of birefringence, leading to an altered probe pulse polarization.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This change in polarization is read out using a balanced detection scheme, consisting of balancing optics (BO), Wollaston prism (WP) and two photodiodes (PD1, PD2).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' B.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Employed pump THz electric field measured using electro-optic sampling.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' C.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Complex refractive index of MAPbBr3 (blue curves) obtained from (10) and Fourier transform of THz field (red area) in B.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A MAPbBr PD1 dwnd ZH BO WP PD2 VIS probezelectricfield(Mv/cm 8 B THz amplitude (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') Re(n) Refractiveindexn 6 Im(n) 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0 0 2 0 2 0 L 2 3 4 5 Time (ps) Freguency(THz)16 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2 | THz-induced birefringence in MAPbBr3 and CsPbBr3 at room temperature.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Room temperature TKE in MAPbBr3 and D.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' CsPbBr3 single crystals.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' B.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' and E.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', THz fluence dependence of transient birefringence peak amplitude with quadratic fit (black line), demonstrating the Kerr effect nature of the signals.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' C.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' and F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', azimuth angle (between probe beam polarization and crystal facets) dependence of main TKE peak with fit (black line) to expected 𝜒(3) tensor geometries in cubic and orthorhombic phase, respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A B c Kerr signal MAPbBr, 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 MAPbBr, 90 peak (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') norr I peak (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') Quadratic fit 135 45 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 THz gence 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 signal 180 0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 ransient 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 Ker 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 225 315 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 2 0 2 4 6 0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 1 270 Time (ps) Max E-field amp.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') Azimuthangle(o)D E F Kerr signal 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 CsPbBr3 90 CsPbBr, peak (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') nori peak (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') Quadratic fit 135 45 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 Jence TH7 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 9 signal 180 0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 ransient 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 Ker 225 315 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 2 0 2 4 6 0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 1 270 Time (ps) Max E-field amp.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') Azimuth angle (°)17 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 3 | TKE temperature dependence of single crystal vs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' thin film MAPbBr3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Temperature-dependent TKE for single crystal and B.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' thin film samples.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' C.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Oscillatory signal components at 80K extracted by subtracting an exponential tail (dashed lines) and starting after the main peak (bottom black arrow) in A, B.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' D.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Respective Fourier transforms (blue and red) of C and incident THz pump spectrum (gray area).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A B c Single crystal Thin film (polycryst.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 80K (Cn 3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 d= 500 μm 3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 d = 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 μm (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 10 latory signal 300K 2.' metadata={'source': 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metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 180K Time (ps) fetbirefr Transient birefr D Transient 80K 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 10 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 80K THz spectrum 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 80K orth.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Spectrum 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 S 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 0 5 10 15 0 5 10 0 1 2 3 4 5 Time (ps) Time(ps) Freguency(THz)18 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 4 | Four-wave mixing simulations vs.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' experimental results in MAPbBr3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Isotropic cubic phase (300 K): Simulated TKE signals for A.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' single crystal (500 µm thickness) and D.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' thin film (400 nm thickness) assuming only instantaneous electronic response 𝑅e(𝑡) (gray lines).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Anisotropic orthorhombic phase (80 K): B.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Single crystal and E.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' thin film TKE vs simulation for model system with static birefringence, instantaneous electronic 𝑅e(𝑡) and Lorentz oscillator 𝑅ph(𝑡) phonon response (purple lines).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' C.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Fourier transforms of experimental data (blue and red) and simulation results (purple) from B.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', E.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', respectively, normalized to the phonon amplitude at 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='15 THz.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A Cubic (300K) B c Orthorhombic (80K) 1.' 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Sim.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' R.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Sim.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' R。' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' + Rph (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') fringence (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0.' 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Thin film Exp.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Thin film S Sim.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' R.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 4 8 Sim.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' R。' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='+ Rph 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 2 0 2 4 6 8 0 5 10 0 1 2 3 4 5 Time (ps) Time (ps) Freauencv(THz)19 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 5 | Nonlinear excitation pathways for the 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='15 THz Raman-active twist mode.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' A.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Time domain coherent phonon oscillations (normalized to 𝑡 = 0 TKE main peak) at 80 K for different THz field strengths (left panel) and respective coherent phonon amplitude (right panel) obtained from Fourier transform;' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' both unveiling a 𝐸THz 2 scaling law and thus demonstrating a nonlinear excitation.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' B.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Possible nonlinear photonic excitation pathways for the 𝜔ph = 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='15 THz mode (dashed line) mediated via a THz electronic polarizability.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The nonlinearly coupled 𝐸THz spectrum (gray area) leads to difference-frequency 𝐸THz𝐸THz ∗ (DF, red area) and sum-frequency 𝐸THz𝐸THz (SF, blue area) driving forces.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The octahedral twist mode is schematically sketched on the right hand side.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' C.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Possible phononic pathways via a directly driven IR-active phonon 𝑄IR, which nonlinearly couples to the Raman-active mode 𝑄𝑅 via anharmonic 𝑄R𝑄IR 2 coupling.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Phonon Amp.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 An (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 0 5 10 15 20 0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 1 Time (ps) B PhotonicPathways 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 EE Driving force 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' VE 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 wn 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4DF SF 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 S EE Wph 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='0 0 1 2 3 4 5 6 Frequency (THz) c Phononic Pathways Difference-frequency Sum-frequency hQIR QIR h2R hIR 0 0 IR-active Raman-active IR-active Raman-active20 Acknowledgments We thank A.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Paarmann, M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Spencer, M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Chergui, A.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Mattoni, and H.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Seiler for fruitful discussion.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Funding: S.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' acknowledges funding for his Emmy Noether group from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation, Nr.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 469405347).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='M and L.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='P acknowledge support of the 2D-HYPE project from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation, Nr.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 490867834) and Agence Nationale de la Recherche (ANR, Nr.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' ANR-21-CE30-0059), respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' XYZ acknowledges support by the Vannevar Bush Faculty Fellowship through Office of Naval Research Grant # N00014-18-1-2080.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='C.' metadata={'source': 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'/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', S.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' contributed theory/analytic tools.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' L.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='H.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' developed FWM model and M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' carried out FWM simulations.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', X.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='-Y.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='Z.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', and S.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' wrote the manuscript.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' All authors read, discussed and commented the manuscript.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='F.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' and M.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='C.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' contributed equally to this work.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Competing interests: The authors declare that they have no competing interests.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Data and materials availability: All data and simulation codes will be uploaded to a public repository after publication of the manuscript.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 21 Supplementary materials Supplementary information 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 CsPbBr3 TKE temperature dependence Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S1 | TKE temperature evolution in CsPbBr3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' TKE in CsPbBr3 at RT and 80K.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In contrast to MAPbBr3, where the structural phase changes for lower temperatures (from cubic to tetragonal to orthorhombic), CsPbBr3 remains in the orthorhombic phase as the temperature is lowered.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This is also reflected in the overall TKE shape.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' However, additional oscillations are visible on the longer timescales at 80K.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Fourier transforming the oscillations after the time indicated by the arrow reveals two main frequency components of 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='9 and 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 THz.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' These frequencies agree well with the two dominating phonon modes in the static Raman spectra of CsPbBr3 (54).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' c, e.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' THz fluence dependence reveals that both oscillation amplitudes (for 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='9 and 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 THz) scale quadratically with the THz electric field.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' d.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Comparison between simulation for an anisotropic material (100 µm thick and 22.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5° azimuthal angle between crystal axis and probe polarization) considering an electronic response only and experimental room temperature CsPbBr3 TKE.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This shows that the complex CsPbBr3 TKE signal may be understood in terms of an instantaneous electronic polarization response alongside anisotropic light propagation.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' u.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='9 2 300K 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 Orth.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' peak ( efringence (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') Spectrum 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 ZHI 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 0 0 1 2 3 Frequency (THz)Transient bire ou Orth (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') (wou) Sim.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' _2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 birefr.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' ak 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 pea 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 ZHI Trans.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='9 0 0 0 5 10 15 20 2 0 2 4 6 8 0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 1 Time (ps) Time (ps)22 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 Estimating the THz nonlinear refractive index of MAPbBr3 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S5 shows a comparison between the TKE in MAPbBr3 and Diamond.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The measured TKE signal strength 𝑆(𝑑) = Δ𝐼/𝐼0, where 𝐼0 is the total probe intensity measured by the photodiodes and Δ𝐼 is the intensity difference, is proportional to Δ𝑛𝜔pr𝑑/𝑐0 in Diamond, where 𝑑 is the sample thickness and 𝜔pr is the probing frequency.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This simple relation holds because there is no significant THz dispersion in Diamond.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' However, due to significant THz absorption and dispersion, this relation does not hold in MAPbBr3 as seen in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S4b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For MAPbBr3, 𝑆(𝑑) may rather be approximated by Δ𝑛𝜔pr 𝑐0 𝑓(𝑑), where 𝑓(𝑑) = ∫ 𝑑𝑧 𝑑 0 ∫ 𝑑𝜔𝐸THz 2 (𝜔)exp(−𝛼(𝜔)𝑧) ∞ 0 / ∫ 𝑑𝜔𝐸THz 2 (𝜔) ∞ 0 .' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S1 Here, 𝐸THz(ω) is the THz pump spectrum and α is the absorption of MAPbBr3 as extracted from the complex refractive index data in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S11.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Since Δ𝑛 = 𝑛2𝑐0𝜖0𝐸THz 2 , we may estimate 𝑛2 of MAPbBr3 using: 𝑛2 MA = 𝑆MA(𝑑MA)𝑑D 𝑆D(𝑑D)𝑓(𝑑MA) 𝑛2 D.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S2 𝑛2 D of Diamond has been measured to be 3 × 10−16 cm2/W for 1 THz pump and 800 nm optical probing (52).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Based on 𝑆MA 𝑆D = 9.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4, 𝑓(𝑑𝑀𝐴 = 500 µm ) = 47µm , we therefore estimate 𝑛2 MA to be 2 × 10−14 cm2/W, roughly 80 times higher than 𝑛2 D for 1 THz pump and 800 nm optical probing.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For comparison, 𝑛2 MA has been previously measured in the near-infrared spectral region using the Z-scan technique (51).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' They found a similar order of magnitude of 𝑛2 MA = 9.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 × 10−14 cm2/W at 1000 nm wavelength.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 23 Supplementary figures Experimental figures Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S2 | MAPbBr3 TKE temporal dependence on THz fluence.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Normalised experimental TKE of MAPbBr3 at RT for various THz fluences showing that the temporal evolution is not affected by the THz-field strength.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 2 in the main text already showed that the 𝑡 = 0 ps peak scales quadratically with the THz field amplitude.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 Max E-Field Amplitude (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='13 Trans.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' birefringence (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='17 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='21 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='26 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='38 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='47 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='56 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='85 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='95 1 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0 2 0 2 4 6 Time (ps)24 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S3 | MAPbBr3 TKE azimuthal angle dependence at RT.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' TKE signal showing the 4- fold rotational symmetry of the measured signal.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b, c.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' TKE signal is normalized to show that the time constant of the tail is independent of azimuthal angle.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This agrees with the simulations for an isotropic material in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S13, where the origin of the exponential tail is high absorption, dispersion and pump-probe walkoff, which do not depend on the crystal azimuthal angle.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Note that the azimuthal angle is not calibrated with respect to the crystal axes in this figure.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b a c Trans.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Transient birefringence (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' u.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') birefringence (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 MAPbBrs (RT) MAPbBr3 (RT) 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='9 Azimuthangle(°) 50 50 10 130 250 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 20 140 260 C 100 C 100 30 150 270 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='7 ngle ngle 40 160 280 150 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 nce 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 50 170 290 150Azimuth 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 Azimuth 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 70 190 310 200 200 80 200 320 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 90 210 330 250 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 250 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 ns.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 100 220 340 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 110 230 350 300 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 120 240 360 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 300 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 0 350 350 1 2 3 0 3 2 0 2 4 1 6 1 2 Time (ps) Time (ps) Time (ps)25 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S4 | MAPbBr3 TKE dependence on sample thickness.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Normalised experimental TKE thickness dependence of MAPbBr3 at RT.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The results agree well with the simulations in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S13.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' shows the measured TKE peak signal as a function of sample thickness.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The black line shows the expected signal dependence when accounting for strong THz absorption and dispersion using the formula 𝑆(𝑑) = ∫ 𝑑𝑧 𝑑 0 ∫ 𝑑𝜔𝐸THz 2 (𝜔)exp(−𝛼(𝜔)𝑧) ∞ 0 / ∫ 𝑑𝑧 1000 0 ∫ 𝑑𝜔𝐸THz 2 (𝜔)exp(−𝛼(𝜔)𝑧) ∞ 0 , where 𝐸𝑇𝐻𝑧(𝜔) is the THz pump spectrum and 𝛼 is the absorption of MAPbBr3 as extracted from the complex refractive index data in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S11.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a b 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 THz field squared d=972μm d=547μm d=132μm 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6birefrin pea 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 TKE 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0 0 2 0 2 4 6 0 200 400 600 800 1000 Time (ps) Thickness d (um)26 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S5 | Comparison between TKE in MAPbBr3 and Diamond for estimating the THz nonlinear refractive index n2.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Diamond has already been shown to have a strong THz-induced Kerr nonlinearity and be a good nonlinear material in the THz range (51).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 𝑛2 of Diamond has been measured to be 3 × 10−16 cm2/W for 1 THz pump and 800 nm optical probing (52).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For a 500 µm thick MAPbBr3 single crystal, the TKE peak signal is about 10 times bigger than for a 400 µm thick Diamond.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' MAPbBr,(d=500um) 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 Transient birefringence ( Diamond (d=400um) 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0 2 0 2 4 Time (ps)27 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S6 | CsPbBr3 TKE azimuthal angle dependence at RT.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Although the main peak exhibits a 4-fold symmetry, the temporal evolution as a function of azimuthal angle is more complex than for MAPbBr3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' As CsPbBr3 is in the orthorhombic phase at room temperature, this extra complexity might be explained by additional static birefringence and resulting anistropic light propagation as can be seen in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S14.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Note that the azimuthal angle is not calibrated with respect to the crystal axes in this figure.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Transient birefringence (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' u.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 50 CsPbBr3 (RT) 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 Azimuth angle (°) 100 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 150 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 200 0 250 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 300 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 350 1 0 1 2 3 Time (ps)28 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S7 | MAPbBr3 TKE at 45° azimuthal angle at 80K.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' MAPbBr3 TKE at 80K for 0° and about 45° azimuthal angle.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' MAPbBr3 is orthorhombic at 80K, which might explain the different overall signal shape for both orientations.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' However, in both TKEs we can see a strong oscillatory signal.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' By subtracting off fits to the tails (dotted line in a) for the TKEs at 0° and 45°, we extract the oscillatory signals.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' c.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Fourier transforming the oscillatory signals in b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' reveals that the same 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 THz mode dominates the oscillatory response at 0° and 45° azimuthal angle.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a b C ingence (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content="5 Azimuth angle (°) ('n 1." metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1THz 0° (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1THz 3 45° 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' ignal 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 mTransient birefr Oscillatory 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 Exponentialfit 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0 5 10 15 20 0 5 10 15 20 0 1 2 3 4 5 Time (ps) Time (ps) Frequency (THz)29 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S8 | Lorentzian fits to spectral peaks in MAPbBr3 at 180K and 80K.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a,c.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=', Oscillatory signals extracted from the MAPbBr3 TKE at 180K and 80K in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 3A respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The signals are extracted by subtracting off exponential fits to the tails from the main TKE signals.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The modulus squared of the Fourier transform of the oscillatory signal at 180K shows a broad peak at 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 THz, which we fit with a Lorentzian.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The FWHM of the Lorentzian amplitude is 𝛥𝜈FWHM =0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='58 THz.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' This corresponds to a phonon lifetime of 𝜏 = 1/(2𝜋𝛥𝜈FWHM ) = 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='27 ps.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' d.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The modulus squared of the Fourier transform of the oscillatory signal at 80K shows two peaks at 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='14 THz and 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='39 THz.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' By fitting Lorentzians, we obtain phonon lifetimes of 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='7(4) ps and 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5(1) ps for the two peaks respectively.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a b X10-3 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 .' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' units) (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' units) MAPbBr3 Single Crystal (180K) Lorentzianfit Wp = 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5THz, 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 Oscillatory signal (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 1 OscillatorModel T = 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='27(5)ps spectrum 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 Power 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0 2 6 0 2 30.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='3 Oscillatory signal (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' units) units MAPbBr3SingleCrystal(80K) Lorentzian fit 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='06 wp = 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='14THz, 2 Oscillator Model t = 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='7(4)ps (arb.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' spectrum 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='04 0 Lorentzian fit Wp = 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='39THz, 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='02 t = 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5(1)ps 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 Power 0 0 5 10 15 20 25 0 2 3 Time (ps) Frequency (THz)30 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S9 | BK7 TKE at room temperature.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' TKE of a BK7 substrate with 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 mm thickness.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' shows the BK7 TKE relative to the TKE of a MAPbBr3 thin film on top of a BK7 substrate with 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 mm thickness at room temperature.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a b X10-3 BK7 (0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5mm) 6 BK7 (0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5mm) MAPbBr3 0n BK7 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 5 (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6Difference 2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 .' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='1 2 0 2 4 6 2 0 2 4 6 Time (ps) Time (ps)31 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S10 | BK7 TKE for various temperatures.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' TKE temperature dependence of BK7 substrate with 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 mm thickness.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' shows the relative strength and shape compared to MAPbBr3 thin film on top of a BK7 substrate for room temperature and 80K.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' BK7 (0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5mm) a b BK7 (0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5mm) 2 MAPbBr3 0on BK7 300K 3.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5(noi 250K 1/IV 2.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Difference signal 145K ransient 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='580K 80K 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0 2 0 2 4 6 0 5 10 Time (ps) Time (ps)32 Simulation figures Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S11 | Dispersion of MAPbBr3 in the THz region.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Refractive index 𝑛 and extinction coefficient 𝜅 of MAPbBr3 calculated using the dielectric function from Sendner et al.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' (10).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Absorption coefficient is calculated using relation 𝛼 = 4𝜋𝜅/𝜆.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The penetration depth is equal to 1/𝛼.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a b 10 1000 6000 5 fficient α (1/cm) oefficient k 5000 Depth (μm) 8 800 e Index n 4 4000 6 600 3Refractiv Extinction Coe 4 400 2 2000 Absorption 2 200 1000 0 0 0 0 0 1 2 3 4 5 0 1 2 3 4 5 Freguency (THz) Freguency(THz)33 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S12 | Extrapolated static birefringence of MAPbBr3 for the simulations of the low temperature orthorhombic phase.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In the optical region, the refractive index of CsPbBr3 is used as measured using the 2D-OKE (46).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The static birefringence of CsPbBr3 is then extrapolated to the THz region.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 𝑛f and 𝑛s correspond to the refractive index along the fast and slow crystal axes and static birefringence is defined as the difference between 𝑛f and 𝑛s.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 8 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='03 Re(n.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') Re(n.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='025 Refractive Index n 6 Birefringence 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='02 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='015 2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='01 0 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='005 0 1 2 3 4 5 Freguency (THz)34 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S13 | Four-wave-mixing simulation for cubic MAPbBr3 for various thicknesses assuming an instantaneous electronic hyperpolarizability response only.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' shows the normalised TKE signal for various thickness.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For thicknesses larger than 100 µm, we can see an exponential tail with a decay time constant largely independent of thickness.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' b.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The normalised TKE signals for various thicknesses are plotted on top of each other.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' On top of the exponential tail, there are small modulations, whose onset depends on the thickness.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The onset time can be roughly estimated by the 𝑡1 time (𝑡1 = (𝑛𝑔,𝑓(𝜔𝑇𝐻𝑧) − 𝑛𝑔,𝑓(𝜔𝑝𝑟))𝑑/𝑐0), where 𝑑 is the sample thickness and 𝑛𝑔 is the group velocity refractive index (40).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a 6 wn006 ringence (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') ringence (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 500μm 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 300μm 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6Transient biret 200μm Transient biref 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 100μm 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4μm 0 0 2 4 6 8 10 2 0 2 4 6 8 10 Time (ps) Time (ps)35 Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S14 | Four-wave-mixing simulation for orthorhombic CsPbBr3 assuming an instantaneous electronic hyperpolarizability response only.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' In contrast to the isotropic simulation in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S13, the azimuthal angle of the model crystal matters for the temporal TKE shape.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' a-d.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Results for 0° azimuthal angle of crystal with respect to probe pulse polarization are shown for various thicknesses.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For this angle, the birefringence experienced by the probe is maximized.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For 0° azimuthal angle and for all thicknesses larger than 200 µm, we can see the appearance of a short-lived oscillatory signal of around 1.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 THz in (a-d).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' These oscillations arise due to static birefringence, but are too short-lived to explain our experimental observation at 80K as shown in (b, d).' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 µm thickness, these oscillations due to static birefringence disappear.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' e-f.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' Results for 45° azimuthal angle for various thicknesses.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' For this angle, the birefringence experienced by the pump is maximized.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The peak t = 0 ps is diminishingly small in comparison to the oscillatory features that happen at later times, which is due to the input tensor symmetry of 𝑅.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The small oscillatory features correspond to internal reflections - similar to the small modulations on top of the tail in Fig.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' S13.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' The onset time for these oscillatory features can be roughly estimated by the 𝑡1 time.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' o° azimuth angle o° azimuth angle a c rans.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' birefringence (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') wno06 Spectrum (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 M 500μm 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 200μm 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4μm0 N.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='W 0 2 0 2 4 6 8 10 0 1 2 3 4 5 Time (ps) Frequency (THz) b d ringence (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') Exp.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' MAPbBr3 Single Crystal (80K) 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 500μm Simulation (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 THzFieldSguared 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6biref 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 Trans.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='5 0 0 5 10 15 0 1 2 3 4 5 Time (ps) Frequency (THz) 45° azimuth angle 45° azimuth angle e MTrans.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=' birefringence (no 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='8 Spectrum (norm.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content=') 500um 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='6 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4 200μm 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='2 0.' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'} +page_content='4um 0 2 0 2 4 6 8 10 0 1 2 3 4 5 Time (ps) Frequency (THz)' metadata={'source': '/home/zjlab/wf/langchain-ChatGLM/knowledge_base/1dE1T4oBgHgl3EQf5AXg/content/2301.03508v1.pdf'}