Preprint PUBDB-2025-00654

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

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2025

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Report No.: arXiv:2502.02343

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 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.

Keyword(s): Materials Science (cond-mat.mtrl-sci) ; Mesoscale and Nanoscale Physics (cond-mat.mes-hall) ; Data Analysis, Statistics and Probability (physics.data-an) ; FOS: Physical sciences


Contributing Institute(s):
  1. CFEL-CMI (FS-CFEL-CMI)
  2. FS-CFEL-1 (Group Leader: Henry Chapman) (CFEL-I)
  3. Computational Nanoscale Imaging (MPSD-CNI)
  4. SPB/SFX (XFEL_E1_SPB/SFX)
  5. The European XFEL Users (XFEL-User)
Research Program(s):
  1. 633 - Life Sciences – Building Blocks of Life: Structure and Function (POF4-633) (POF4-633)
  2. AIM, DFG project G:(GEPRIS)390715994 - EXC 2056: CUI: Advanced Imaging of Matter (390715994) (390715994)
Experiment(s):
  1. SPB: Single Particles, clusters & Biomolecules (SASE1)

Appears in the scientific report 2025
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Creative Commons Attribution CC BY 4.0 ; OpenAccess
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Private Collections > >CFEL > >FS-CFEL > CFEL-I
Private Collections > >DESY > >FS > FS-CFEL-CMI
Private Collections > >XFEL.EU > XFEL_E1_SPB/SFX
Private Collections > >XFEL.EU > XFEL-User
Private Collections > >MPG > MPSD-CNI
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 Record created 2025-02-05, last modified 2025-03-10