Decoding ultrafast polarization responses in lead halide perovskites by the two-dimensional optical Kerr effect

Maehrlein, Sebastian F.; Joshi, Prakriti P.; Huber, Lucas; Wang, Feifan; Cherasse, Marie; Liu, Yufeng; Juraschek, Dominik M.; Mosconi, Edoardo; Meggiolaro, Daniele; De Angelis, Filippo; Zhu, X. -Y.

doi:10.1073/pnas.2022268118

DOE OSTI · 1765015

Decoding ultrafast polarization responses in lead halide perovskites by the two-dimensional optical Kerr effect

Maehrlein, Sebastian F.·Joshi, Prakriti P.·Huber, Lucas·Wang, Feifan·Cherasse, Marie·Liu, Yufeng·Juraschek, Dominik M.·Mosconi, Edoardo·Meggiolaro, Daniele·De Angelis, Filippo·Zhu, X. -Y.

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Abstract

Significance Optoelectronic devices, such as photovoltaics or light-emitting diodes, are based on the interaction of light with charges in the active material. Lead halide perovskites (LHPs) have emerged as excellent materials for optoelectronics, but mysteries remain as to how these materials interact with light. Here, we develop a spectroscopic method to observe the nearly instantaneous responses of LHPs to propagating light fields. This method has allowed us to precisely trace a nonlinear material response resulting from the mixing of different light components overtaking each other during propagation. The resulting oscillatory signals could be easily confused with collective motions of ions or molecules, but are quantitatively accounted by strong nonlinear mixing and polarization-dressed light propagation in single-crystal LHPs.

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14 SOLAR ENERGY 36 MATERIALS SCIENCE 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY 42 ENGINEERING Science & Technology - Other Topics four-wave mixing lead halide perovskites light propagation multidimensional coherent spectroscopy nonlinear polarization

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Maehrlein, Sebastian F., Joshi, Prakriti P., Huber, Lucas, Wang, Feifan, Cherasse, Marie, Liu, Yufeng, Juraschek, Dominik M., Mosconi, Edoardo, Meggiolaro, Daniele, De Angelis, Filippo, Zhu, X. -Y.. 2021-02-08. Decoding ultrafast polarization responses in lead halide perovskites by the two-dimensional optical Kerr effect. https://doi.org/10.1073/pnas.2022268118

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