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PreprintCC BY 4.0arXiv

Intensity-driven Mott-like transition in a 2D Ruddlesden-Popper perovskite

Abstract

Two-dimensional Ruddlesden-Popper-type halide perovskites have emerged as promising cutting-edge nonlinear optical materials due to their strong excitonic effects and carrier-density-dependent optical responses. In this work, we investigate the nonlinear optical properties and ultrafast carrier dynamics of (BA)2PbI4 under infrared excitation, resonant with the two-photon energy of its excitonic transition. Using a nonlinear femtosecond Z-scan measurement with a 1030\,nm pump pulse, we observe a pronounced intensity-dependent evolution of the nonlinear absorption coefficient and the refractive index. With increasing pump intensity, a switch from saturable absorption to reverse saturable absorption emerges, suggesting an intensity-driven Mott-like transition. To elucidate the underlying carrier dynamics, intensity-dependent transient absorption spectroscopy was performed under the same excitation intensities. This reveals a long-lived charge carrier population above the estimated Mott density, reflecting a clear phase transition from an exciton-dominated regime to a dense electron-hole plasma regime. Moreover, such an intensity-driven, high, and switchable nonlinear optical response, along with a Mott-like transition under infrared pulse excitation, makes the 2D (BA)2PbI4 perovskites suitable for all-optical operation in the infrared regime.

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BibTeX
@misc{mondal2026intensitydriven,
  title = {{Intensity-driven Mott-like transition in a 2D Ruddlesden-Popper perovskite}},
  author = {Koushik Mondal and Amit Haldar and Indrajit Mondal and Arpita Dutta and Himanshu Bhatt and Biswajit Mahata and Soumili Banerjee and Hirendra Nath Ghosh and Satyaprasad P Senanayak and Shovon Pal},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2610.30964},
  eprint = {2610.30964},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2610.30964},
  note = {CC BY 4.0},
}
RIS
TY  - UNPB
TI  - Intensity-driven Mott-like transition in a 2D Ruddlesden-Popper perovskite
AU  - Koushik Mondal
AU  - Amit Haldar
AU  - Indrajit Mondal
AU  - Arpita Dutta
AU  - Himanshu Bhatt
AU  - Biswajit Mahata
AU  - Soumili Banerjee
AU  - Hirendra Nath Ghosh
AU  - Satyaprasad P Senanayak
AU  - Shovon Pal
PY  - 2026
DA  - 2026/10/22
PB  - arXiv
DO  - 10.48550/arxiv.2610.30964
UR  - https://arxiv.org/abs/2610.30964
AB  - Two-dimensional Ruddlesden-Popper-type halide perovskites have emerged as promising cutting-edge nonlinear optical materials due to their strong excitonic effects and carrier-density-dependent optical responses. In this work, we investigate the nonlinear optical properties and ultrafast carrier dynamics of (BA)_2PbI_4 under infrared excitation, resonant with the two-photon energy of its excitonic transition. Using a nonlinear femtosecond Z-scan measurement with a 1030\,nm pump pulse, we observe a pronounced intensity-dependent evolution of the nonlinear absorption coefficient and the refractive index. With increasing pump intensity, a switch from saturable absorption to reverse saturable absorption emerges, suggesting an intensity-driven Mott-like transition. To elucidate the underlying carrier dynamics, intensity-dependent transient absorption spectroscopy was performed under the same excitation intensities. This reveals a long-lived charge carrier population above the estimated Mott density, reflecting a clear phase transition from an exciton-dominated regime to a dense electron-hole plasma regime. Moreover, such an intensity-driven, high, and switchable nonlinear optical response, along with a Mott-like transition under infrared pulse excitation, makes the 2D (BA)_2PbI_4 perovskites suitable for all-optical operation in the infrared regime.
ER  -