Efficient up-conversion in CsPbBr3 nanocrystals via phonon-driven exciton-polaron formation

Abdullah S. Abbas, Beiye C. Li, Richard D. Schaller, Vitali B. Prakapenka, Stella Chariton, Daqian Bian, Gregory S. Engel and A. Paul Alivisatos ()
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Abdullah S. Abbas: Berkeley
Beiye C. Li: The University of Chicago
Richard D. Schaller: Northwestern University
Vitali B. Prakapenka: The University of Chicago
Stella Chariton: The University of Chicago
Daqian Bian: The University of Chicago
Gregory S. Engel: The University of Chicago
A. Paul Alivisatos: Berkeley

Nature Communications, 2025, vol. 16, issue 1, 1-8

Abstract: Abstract Lead halide perovskite nanocrystals demonstrate efficient up-conversion, although the precise mechanism remains a subject of active research. This study utilizes steady-state and time-resolved spectroscopy methods to unravel the mechanism driving the up-conversion process in CsPbBr3 nanocrystals. Employing above- and below-gap photoluminescence measurements, we extract a distinct phonon mode with an energy of ~7 meV and identify the Pb-Br-Pb bending mode as the phonon involved in the up-conversion process. This result was corroborated by Raman spectroscopy. We confirm an up-conversion efficiency reaching up to 75%. Transient absorption measurements under conditions of sub-gap excitation also unexpectedly reveal coherent phonons for the subset of nanocrystals undergoing up-conversion. This coherence implies that the up-conversion and subsequent relaxation is accompanied by a synchronized and phased lattice motion. This study reveals that efficient up-conversion in CsPbBr3 nanocrystals is powered by a unique interplay between the soft lattice structure, phonons, and excited states dynamics.

Date: 2025
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DOI: 10.1038/s41467-025-60992-y

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