Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite

Zhang, Zhuquan; Zhang, Jiahao; Liu, Zi-Jie; Dahodl, Nabeel S.; Paritmongkol, Watcharaphol; Niamh, Brown,; Yu-Che, Chien,; Dai, Zhenbang; Nelson, Keith A.; Tisdale, William A.; Rappe, Andrew M.; Baldini, Edoardo

doi:10.48550/arxiv.2301.03501

Cited by 1 publication

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References 47 publications

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“…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 an SF nonlinear photonic mechanism. We leave the determination of the exact excitation pathway to further studies, e.g., by 2D THz spectroscopy (54) or more narrowband THz excitation (55).…”

Section: Discussionmentioning

confidence: 99%

Nonlinear terahertz control of the lead halide perovskite lattice

et al. 2023

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Lead halide perovskites (LHPs) have emerged as an excellent class of semiconductors for next-generation solar cells and optoelectronic devices. Tailoring physical properties by fine-tuning the lattice structures has been explored in these materials by chemical composition or morphology. Nevertheless, its dynamic counterpart, phonon-driven ultrafast material control, as contemporarily harnessed for oxide perovskites, has not yet been established. Here, we use intense THz electric fields to obtain direct lattice control via nonlinear excitation of coherent octahedral twist modes in hybrid CH 3 NH 3 PbBr 3 and all-inorganic CsPbBr 3 perovskites. These Raman-active phonons at 0.9 to 1.3 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. Our work opens the door to selective control of LHP’s vibrational degrees of freedom governing phase transitions and dynamic disorder.

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Section: Discussionmentioning

confidence: 99%