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

Abstract

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, anmore » 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.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1296683
Report Number(s):
LA-UR-16-21000
Journal ID: ISSN 1530-6984
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 16; Journal Issue: 4; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; material Science; Cs-Pb-halide perovskites; nanocrystal; quantum dot; radiative recombination; Auger recombination; absorption cross-section; band-edge-state degeneracy; intraband cooling; exciton-exciton interaction

Citation Formats

Makarov, Nikolay Sergeevich, Guo, Shaojun, Isaienko, Oleksandr, Liu, Wenyong, Robel, Istvan, and Klimov, Victor Ivanovich. Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots. United States: N. p., 2016. Web. doi:10.1021/acs.nanolett.5b05077.
Makarov, Nikolay Sergeevich, Guo, Shaojun, Isaienko, Oleksandr, Liu, Wenyong, Robel, Istvan, & Klimov, Victor Ivanovich. Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots. United States. doi:10.1021/acs.nanolett.5b05077.
Makarov, Nikolay Sergeevich, Guo, Shaojun, Isaienko, Oleksandr, Liu, Wenyong, Robel, Istvan, and Klimov, Victor Ivanovich. Tue . "Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots". United States. doi:10.1021/acs.nanolett.5b05077. https://www.osti.gov/servlets/purl/1296683.
@article{osti_1296683,
title = {Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots},
author = {Makarov, Nikolay Sergeevich and Guo, Shaojun and Isaienko, Oleksandr and Liu, Wenyong and Robel, Istvan and Klimov, Victor Ivanovich},
abstractNote = {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.},
doi = {10.1021/acs.nanolett.5b05077},
journal = {Nano Letters},
issn = {1530-6984},
number = 4,
volume = 16,
place = {United States},
year = {2016},
month = {2}
}

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