Resonant Multiple-Phonon Absorption Causes Efficient Anti-Stokes Photoluminescence in CsPbBr 3 Nanocrystals

Lead halide perovskite nanocrystals, such as CsPbBr , exhibit efficient photoluminescence (PL) up-conversion, also referred to as anti-Stokes photoluminescence (ASPL). This is a phenomenon where irradiating nanocrystals up to 100 meV below gap results in higher energy band edge emission. Most surpri...

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Bibliographic Details
Published in:ACS nano 2024-02, Vol.18 (8), p.6438-6444
Main Authors: Zhang, Zhuoming, Ghonge, Sushrut, Ding, Yang, Zhang, Shubin, Berciu, Mona, Schaller, Richard D, Jankó, Boldizsár, Kuno, Masaru
Format: Article
Language:English
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Summary:Lead halide perovskite nanocrystals, such as CsPbBr , exhibit efficient photoluminescence (PL) up-conversion, also referred to as anti-Stokes photoluminescence (ASPL). This is a phenomenon where irradiating nanocrystals up to 100 meV below gap results in higher energy band edge emission. Most surprising is that ASPL efficiencies approach unity and involve single-photon interactions with multiple phonons. This is unexpected given the statistically disfavored nature of multiple-phonon absorption. Here, we report and rationalize near-unity anti-Stokes photoluminescence efficiencies in CsPbBr nanocrystals and attribute them to resonant multiple-phonon absorption by polarons. The theory explains paradoxically large efficiencies for intrinsically disfavored, multiple-phonon-assisted ASPL in nanocrystals. Moreover, the developed microscopic mechanism has immediate and important implications for applications of ASPL toward condensed phase optical refrigeration.
ISSN:1936-0851
1936-086X
DOI:10.1021/acsnano.3c11908