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Direct observation of the exciton polaron by serial femtosecond crystallography on single CsPbBr$_3$ quantum dots

Direct observation of the exciton polaron by serial femtosecond crystallography on single CsPbBr$_3$ quantum dots

来源:Arxiv_logoArxiv
英文摘要

The outstanding opto-electronic properties of lead halide perovskites have been related to the formation of polarons. Nevertheless, the observation of the atomistic deformation brought about by one electron-hole pair in these materials has remained elusive. Here, we measure the diffraction patterns of single CsPbBr$_3$ quantum dots (QDs) with and without resonant excitation in the single exciton limit using serial femtosecond crystallography (SFX). By reconstructing the 3D differential diffraction pattern, we observe small shifts of the Bragg peaks indicative of a crystal-wide deformation field. Building on DFT calculations, we show that these shifts are consistent with the lattice distortion induced by a delocalized electron and a localized hole, forming a mixed large/small exciton polaron. This result creates a clear picture of the polaronic deformation in CsPbBr$_3$ QDs, highlights the exceptional sensitivity of SFX to lattice distortions in few-nanometer crystallites, and establishes an experimental platform for future studies of electron-lattice interactions.

Grant Mills、Tokushi Sato、Safi Rafie-Zinedine、Yulong Zhuang、Johan Bielecki、Henry N. Chapman、Juncheng E、Kartik Ayyer、Adrian P. Mancuso、Zeger Hens、Onur Erdem、Diogo Melo、Jochen K¨1pper、Lena Worbs、Raphael de Wijn、Margarita Samoli、Jayanath Koliyadu、Holger Lange、Amit Kumar Samanta、Yoonhee Kim、Jannik L¨1bke、Adam Round、Federico Locardi、Ivan Infante、Tamme Wollweber、Richard Bean、Zhou Shen、Abhishek Mall、Romain Letrun、Chan Kim、Armando Estillore

物理学晶体学

Grant Mills,Tokushi Sato,Safi Rafie-Zinedine,Yulong Zhuang,Johan Bielecki,Henry N. Chapman,Juncheng E,Kartik Ayyer,Adrian P. Mancuso,Zeger Hens,Onur Erdem,Diogo Melo,Jochen K¨1pper,Lena Worbs,Raphael de Wijn,Margarita Samoli,Jayanath Koliyadu,Holger Lange,Amit Kumar Samanta,Yoonhee Kim,Jannik L¨1bke,Adam Round,Federico Locardi,Ivan Infante,Tamme Wollweber,Richard Bean,Zhou Shen,Abhishek Mall,Romain Letrun,Chan Kim,Armando Estillore.Direct observation of the exciton polaron by serial femtosecond crystallography on single CsPbBr$_3$ quantum dots[EB/OL].(2025-02-04)[2025-08-02].https://arxiv.org/abs/2502.02343.点此复制

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