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Polaron-Enhanced Polariton Nonlinearity in Lead Halide Perovskites

机译:卤化铅钙钛矿中的极化子增强极化激元非线性

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摘要

Exciton-polaritons offer a versatile platform for realization of all-optical integrated logic gates due to the strong effective optical nonlinearity resulting from the exciton-exciton interactions. In most of the current excitonic materials there exists a direct connection between the exciton robustness to thermal fluctuations and the strength of the exciton-exciton interaction, making materials with the highest levels of exciton nonlinearity applicable at cryogenic temperatures only. Here, we show that strong polaronic effects, characteristic for perovskite materials, allow overcoming this limitation. Namely, we demonstrate a record-high value of the nonlinear optical response in the nanostructured organic-inorganic halide perovskite MAPbI3, experimentally detected as a 19.7 meV blueshift of the polariton branch under femtosecond laser irradiation. This is substantially higher than characteristic values for the samples based on conventional semiconductors and monolayers of transition-metal dichalcogenides. The observed strong polaron-enhanced nonlinearity exists for both tetragonal and orthorhombic phases of MAPbI3 and remains stable at elevated temperatures.
机译:激子-极化激元为实现全光集成逻辑门提供了一个多功能平台,因为激子-激子相互作用会产生强大的有效光学非线性。在目前的大多数激子材料中,激子对热波动的鲁棒性与激子-激子相互作用的强度之间存在直接联系,因此具有最高水平激子非线性的材料仅适用于低温。在这里,我们表明钙钛矿材料所特有的强极化效应可以克服这一限制。也就是说,我们证明了纳米结构有机-无机卤化物钙钛矿MAPbI3的非线性光学响应值创历史新高,实验检测到飞秒激光照射下极化激元分支的19.7 meV蓝移。这大大高于基于传统半导体和过渡金属硫族化合物单层样品的特征值。观察到的强极化子增强非线性存在于 MAPbI3 的四方相和斜方相中,并且在高温下保持稳定。

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