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Second-order Raman and anharmonic lattice dynamics in lead-halide perovskites

Abstract

We explore the microscopic origin of THz-driven lattice dynamics in methylammonium lead bromide CH3NH3PbBr3 using two-dimensional THz Kerr-effect spectroscopy. The analysis of the experiment enables discrimination between competing nonlinear excitation mechanisms and reveals that the dominant pathway is phonon-mediated rather than purely photonic. In particular, we argue that the commonly observed 1.15~THz Raman-active Ag mode is not excited directly by the THz electric field. Instead, it emerges through cubic anharmonic coupling to an infrared-active phonon at 0.68~THz. Furthermore, a satellite feature at 1.36~THz is identified as a two-phonon Raman response of the same infrared-active mode. The observation of strong quadratic coupling involving the infrared-active phonon suggests an unconventional form of electron-phonon dressing present in lead-halide perovskites.

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BibTeX
@misc{shen2026secondorder,
  title = {{Second-order Raman and anharmonic lattice dynamics in lead-halide perovskites}},
  author = {Chao Shen and Florian Kluibenschedl and Ayan A. Zhumekenov and Mikhail Lemeshko and Osman M. Bakr and Artem G. Volosniev and Zhanybek Alpichshev},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2610.03274},
  eprint = {2610.03274},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2610.03274},
}
RIS
TY  - UNPB
TI  - Second-order Raman and anharmonic lattice dynamics in lead-halide perovskites
AU  - Chao Shen
AU  - Florian Kluibenschedl
AU  - Ayan A. Zhumekenov
AU  - Mikhail Lemeshko
AU  - Osman M. Bakr
AU  - Artem G. Volosniev
AU  - Zhanybek Alpichshev
PY  - 2026
DA  - 2026/10/02
PB  - arXiv
DO  - 10.48550/arxiv.2610.03274
UR  - https://arxiv.org/abs/2610.03274
AB  - We explore the microscopic origin of THz-driven lattice dynamics in methylammonium lead bromide CH_3NH_3PbBr_3 using two-dimensional THz Kerr-effect spectroscopy. The analysis of the experiment enables discrimination between competing nonlinear excitation mechanisms and reveals that the dominant pathway is phonon-mediated rather than purely photonic. In particular, we argue that the commonly observed 1.15~THz Raman-active A_g mode is not excited directly by the THz electric field. Instead, it emerges through cubic anharmonic coupling to an infrared-active phonon at 0.68~THz. Furthermore, a satellite feature at 1.36~THz is identified as a two-phonon Raman response of the same infrared-active mode. The observation of strong quadratic coupling involving the infrared-active phonon suggests an unconventional form of electron-phonon dressing present in lead-halide perovskites.
ER  -