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Direct observation of the exciton polaron by serial femtosecond crystallography on single CsPbBr₃ quantum dots

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arxiv 2502.02343 v1 pith:GEQP2HT2 submitted 2025-02-04 cond-mat.mtrl-sci cond-mat.mes-hallphysics.data-an

Direct observation of the exciton polaron by serial femtosecond crystallography on single CsPbBr₃ quantum dots

classification cond-mat.mtrl-sci cond-mat.mes-hallphysics.data-an
keywords cspbbrdeformationexcitonsinglecrystallographydiffractiondotsfemtosecond
verification ladder T0 review T1 audit T2 compute T3 formal T4 reserved
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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.

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