ACS Nano, volume 14, issue 11, pages 14939-14946
Unraveling the Origin of the Long Fluorescence Decay Component of Cesium Lead Halide Perovskite Nanocrystals
Michael A Becker
1, 2
,
Caterina Bernasconi
3, 4
,
Maryna I. Bodnarchuk
3, 4
,
G. Rainò
3, 4
,
Maksym V. Kovalenko
3, 4
,
David J Norris
2
,
Rainer F. Mahrt
1
,
Thilo Stöferle
1
1
IBM Research Europe−Zurich, Säumerstrasse 4, 8803 Rüschlikon, Switzerland
|
Publication type: Journal Article
Publication date: 2020-11-11
PubMed ID:
33174717
General Physics and Astronomy
General Materials Science
General Engineering
Abstract
A common signature of nearly all nanoscale emitters is fluorescence intermittency, which is a rapid switching between “on”-states exhibiting a high photon emission rate and “off”-states with a much lower rate. One consequence of fluorescence intermittency occurring on time scales longer than the exciton decay time is the so-called delayed photon emission, manifested by a long radiative decay component. Besides their dominant fast radiative decay, fully inorganic cesium lead halide perovskite quantum dots exhibit a long fluorescence decay component at cryogenic temperatures that is often attributed to the decay of the dark exciton. Here, we show that its origin is delayed photon emission by investigating temporal variations in fluorescence intensity and concomitant decay times found in single CsPbBr3 perovskite quantum dots. We attribute the different intensity levels of the intensity trace to a rapid switching between a high-intensity exciton state and an Auger-reduced low-intensity trion state that occurs when the excitation is sufficiently strong. Surprisingly, we observe that the exponent of this power-law-dependent delayed emission is correlated with the emission intensity, which cannot be explained with existing charge carrier trapping models. Our analysis reveals that the long decay component is mainly governed by delayed emission, which is present in both the exciton and trion state. The absence of a fine structure in trions clarifies the vanishing role of the dark exciton state for the long decay component. Our findings are essential for the development of a complete photophysical model that captures all observed features of fluorescence variations in colloidal nanocrystals.
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1
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Citations by publishers
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2
4
6
8
10
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10 publications, 40%
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7 publications, 28%
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1 publication, 4%
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1 publication, 4%
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1 publication, 4%
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2
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10
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- We do not take into account publications without a DOI.
- Statistics recalculated only for publications connected to researchers, organizations and labs registered on the platform.
- Statistics recalculated weekly.
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Becker M. A. et al. Unraveling the Origin of the Long Fluorescence Decay Component of Cesium Lead Halide Perovskite Nanocrystals // ACS Nano. 2020. Vol. 14. No. 11. pp. 14939-14946.
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Becker M. A., Bernasconi C., Bodnarchuk M. I., Rainò G., Kovalenko M. V., Norris D. J., Mahrt R. F., Stöferle T. Unraveling the Origin of the Long Fluorescence Decay Component of Cesium Lead Halide Perovskite Nanocrystals // ACS Nano. 2020. Vol. 14. No. 11. pp. 14939-14946.
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TY - JOUR
DO - 10.1021/acsnano.0c04401
UR - https://doi.org/10.1021/acsnano.0c04401
TI - Unraveling the Origin of the Long Fluorescence Decay Component of Cesium Lead Halide Perovskite Nanocrystals
T2 - ACS Nano
AU - Bernasconi, Caterina
AU - Becker, Michael A
AU - Bodnarchuk, Maryna I.
AU - Rainò, G.
AU - Kovalenko, Maksym V.
AU - Norris, David J
AU - Mahrt, Rainer F.
AU - Stöferle, Thilo
PY - 2020
DA - 2020/11/11 00:00:00
PB - American Chemical Society (ACS)
SP - 14939-14946
IS - 11
VL - 14
PMID - 33174717
SN - 1936-0851
SN - 1936-086X
ER -
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@article{2020_Becker,
author = {Caterina Bernasconi and Michael A Becker and Maryna I. Bodnarchuk and G. Rainò and Maksym V. Kovalenko and David J Norris and Rainer F. Mahrt and Thilo Stöferle},
title = {Unraveling the Origin of the Long Fluorescence Decay Component of Cesium Lead Halide Perovskite Nanocrystals},
journal = {ACS Nano},
year = {2020},
volume = {14},
publisher = {American Chemical Society (ACS)},
month = {nov},
url = {https://doi.org/10.1021/acsnano.0c04401},
number = {11},
pages = {14939--14946},
doi = {10.1021/acsnano.0c04401}
}
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Becker, Michael A., et al. “Unraveling the Origin of the Long Fluorescence Decay Component of Cesium Lead Halide Perovskite Nanocrystals.” ACS Nano, vol. 14, no. 11, Nov. 2020, pp. 14939-14946. https://doi.org/10.1021/acsnano.0c04401.