Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots

Makarov, Nikolay Sergeevich; Guo, Shaojun; Isaienko, Oleksandr; Liu, Wenyong; Robel, Istvan; Klimov, Victor Ivanovich

doi:10.1021/acs.nanolett.5b05077

Title: Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots

Journal Article · Tue Feb 16 00:00:00 EST 2016 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.5b05077· OSTI ID:1296683

Makarov, Nikolay Sergeevich ^[1]; Guo, Shaojun ^[1]; Isaienko, Oleksandr ^[1]; Liu, Wenyong ^[1]; Robel, Istvan ^[1]; Klimov, Victor Ivanovich ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Organic–inorganic lead-halide perovskites have been the subject of recent intense interest due to their unusually strong photovoltaic performance. A new addition to the perovskite family is all-inorganic Cs–Pb-halide perovskite nanocrystals, or quantum dots, fabricated via a moderate-temperature colloidal synthesis. While being only recently introduced to the research community, these nanomaterials have already shown promise for a range of applications from color-converting phosphors and light-emitting diodes to lasers, and even room-temperature single-photon sources. Knowledge of the optical properties of perovskite quantum dots still remains vastly incomplete. Here we apply various time-resolved spectroscopic techniques to conduct a comprehensive study of spectral and dynamical characteristics of single- and multiexciton states in CsPbX3 nanocrystals with X being either Br, I, or their mixture. Specifically, we measure exciton radiative lifetimes, absorption cross-sections, and derive the degeneracies of the band-edge electron and hole states. We also characterize the rates of intraband cooling and nonradiative Auger recombination and evaluate the strength of exciton–exciton coupling. The overall conclusion of this work is that spectroscopic properties of Cs–Pb-halide quantum dots are largely similar to those of quantum dots of more traditional semiconductors such as CdSe and PbSe. At the same time, we observe some distinctions including, for example, an appreciable effect of the halide identity on radiative lifetimes, considerably shorter biexciton Auger lifetimes, and apparent deviation of their size dependence from the “universal volume scaling” previously observed for many traditional nanocrystal systems. The high efficiency of Auger decay in perovskite quantum dots is detrimental to their prospective applications in light-emitting devices and lasers. Furthermore, this points toward the need for the development of approaches for effective suppression of Auger recombination in these nanomaterials, using perhaps insights gained from previous studies of II–VI nanocrystals.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1296683

Report Number(s):: LA-UR-16-21000

Journal Information:: Nano Letters, Vol. 16, Issue 4; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 470 works

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Metal Halide Perovskite Nanocrystals: Synthesis, Post-Synthesis Modifications and Their Optical Properties Shamsi, Javad; Urban, Alexander S.; Imran, Muhammad arXiv https://doi.org/10.48550/arxiv.2010.14939	text	January 2020

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
material Science
Cs-Pb-halide perovskites
nanocrystal
quantum dot
radiative recombination
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absorption cross-section
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Title: Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots

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