Direct observation of the exciton polaron by serial femtosecond crystallography on single CsPbBr3 quantum dots
Authors
Zhou Shen, Margarita Samoli, Onur Erdem, Johan Bielecki, Amit Kumar Samanta, Juncheng E, Armando Estillore, Chan Kim, Yoonhee Kim, Jayanath Koliyadu, Romain Letrun, Federico Locardi, Jannik Lübke, Abhishek Mall, Diogo Melo, Grant Mills, Safi Rafie-Zinedine, Adam Round, Tokushi Sato, Raphael de Wijn, Tamme Wollweber, Lena Worbs, Yulong Zhuang, Adrian P. Mancuso, Richard Bean, Henry N. Chapman, Jochen Küpper, Ivan Infante, Holger Lange, Zeger Hens and Kartik Ayyer
Abstract
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 CsPbBr3 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 CsPbBr3 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.