Chemistry of Materials, volume 33, issue 9, pages 3349-3358
Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence
Publication type: Journal Article
Publication date: 2021-04-21
Journal:
Chemistry of Materials
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor: 8.6
ISSN: 08974756, 15205002
Materials Chemistry
General Chemistry
General Chemical Engineering
Abstract
Trap states play a crucial role in the design of colloidal quantum dot (QD)-based technologies. The presence of these in-gap states can either significantly limit the efficiency of devices (e.g., in solar cells or LEDs) or play a pivotal role in the functioning of the technology (e.g., in catalysis). Understanding the atomistic nature of traps is therefore of the highest importance. Although the mechanism through which undercoordinated chalcogenide atoms can lead to trap states in II–VI QDs is generally well understood, the nature of metal-based traps remains more elusive. Previous research has shown that reduction of metal sites in negatively charged QDs can lead to in-gap states. Here, we use density functional theory to show that metal-based traps are also formed in charge-neutral but photoexcited CdSe QDs. It is found that Cd–Cd dimers and the concomitant trap states are transient in nature and appear and disappear on the picosecond time scale. Subsequent nonradiative recombination from the trap is shown to be much faster than radiative recombination, indicating that dimer-related trap states can quench the photoluminescence. These results are expected to be transferable to other II–VI materials and highlight the importance of surface redox reactions for the optical properties of QDs. Moreover, they show that photoexcitation can lead to atomic rearrangements on the surface and thus create transient in-gap states.
Top-30
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1 publication, 4%
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Citations by publishers
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17 publications, 68%
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2 publications, 8%
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Wiley
1 publication, 4%
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1 publication, 4%
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Multidisciplinary Digital Publishing Institute (MDPI)
1 publication, 4%
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Elsevier
1 publication, 4%
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1 publication, 4%
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1 publication, 4%
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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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Du Fossé I. et al. Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence // Chemistry of Materials. 2021. Vol. 33. No. 9. pp. 3349-3358.
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Du Fossé I., Boehme S. C., Infante I., Houtepen A. Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence // Chemistry of Materials. 2021. Vol. 33. No. 9. pp. 3349-3358.
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TY - JOUR
DO - 10.1021/acs.chemmater.1c00561
UR - https://doi.org/10.1021/acs.chemmater.1c00561
TI - Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence
T2 - Chemistry of Materials
AU - Du Fossé, Indy
AU - Boehme, Simon C
AU - Infante, Ivan
AU - Houtepen, A.J
PY - 2021
DA - 2021/04/21 00:00:00
PB - American Chemical Society (ACS)
SP - 3349-3358
IS - 9
VL - 33
SN - 0897-4756
SN - 1520-5002
ER -
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@article{2021_Du Fossé,
author = {Indy Du Fossé and Simon C Boehme and Ivan Infante and A.J Houtepen},
title = {Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence},
journal = {Chemistry of Materials},
year = {2021},
volume = {33},
publisher = {American Chemical Society (ACS)},
month = {apr},
url = {https://doi.org/10.1021/acs.chemmater.1c00561},
number = {9},
pages = {3349--3358},
doi = {10.1021/acs.chemmater.1c00561}
}
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Du Fossé, Indy, et al. “Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence.” Chemistry of Materials, vol. 33, no. 9, Apr. 2021, pp. 3349-3358. https://doi.org/10.1021/acs.chemmater.1c00561.