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

Abbas, Abdullah S.; Li, Beiye C.; Schaller, Richard D.; Prakapenka, Vitali B.; Chariton, Stella; Bian, Daqian; Engel, Gregory S.; Alivisatos, A. Paul

doi:10.1038/s41467-025-60992-y

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

Journal Article · Tue Jul 01 00:00:00 UTC 2025 · Nature Communications

DOI: https://doi.org/10.1038/s41467-025-60992-y · OSTI ID:2588215

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^[2]; Schaller, Richard D. ^[3];

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^[2]; Alivisatos, A. Paul ^[4]

University of California, Berkeley, CA (United States); University of Chicago, IL (United States)
University of Chicago, IL (United States)
Northwestern University, Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
University of California, Berkeley, CA (United States); University of Chicago, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); Samsung Advanced Institute of Technology (SAIT); US Department of Energy; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences & Biosciences Division (SC-22.1); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 2588215

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723

Publisher:: Springer Science and Business Media LLCCopyright Statement

Country of Publication:: United States

Language:: English

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