Suppressing Non‐Radiative Relaxation through Single‐Atom Metal Modification for Enhanced Fluorescence Efficiency in Molybdenum Disulfide Quantum Dots

To enhance the fluorescence efficiency of semiconductor nanocrystal quantum dots (QDs), strategies via enhancing photo‐absorption and eliminating non‐radiative relaxation have been proposed. In this study, we demonstrate that fluorescence efficiency of molybdenum disulfide quantum dots (MoS2 QDs) ca...

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Published in:Angewandte Chemie International Edition 2022-08, Vol.61 (34), p.e202207300-n/a
Main Authors: Li, Chao‐Rui, Lei, Yu‐Li, Li, Hua, Ni, Miao, Yang, Dong‐Rui, Xie, Xiao‐Yu, Wang, Yuan‐Fan, Ma, Hai‐Bo, Xu, Wei‐Gao, Xia, Xing‐Hua
Format: Article
Language:English
Subjects:
Atomically Dispersed Metals
Conduction bands
Copper
Efficiency
Electrons
Energy levels
Fluorescence
Fluorescence Enhancement
Forbidden bands
Gold
Heavy metals
Metals
Molybdenum
Molybdenum Disulfide
Nanocrystals
Non-Radiative Recombination
Quantum Dots
Recombination
Silver
Valence band
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Summary:To enhance the fluorescence efficiency of semiconductor nanocrystal quantum dots (QDs), strategies via enhancing photo‐absorption and eliminating non‐radiative relaxation have been proposed. In this study, we demonstrate that fluorescence efficiency of molybdenum disulfide quantum dots (MoS2 QDs) can be enhanced by single‐atom metal (Au, Ag, Pt, Cu) modification. Four‐fold enhancement of the fluorescence emission of MoS2 QDs is observed with single‐atom Au modification. The underlying mechanism is ascribed to the passivation of non‐radiative surface states owing to the new defect energy level of Au in the forbidden band that can trap excess electrons in n‐type MoS2, increasing the recombination probability of conduction band electrons with valence band holes of MoS2. Our results open an avenue for enhancing the fluorescence efficiency of QDs via the modification of atomically dispersed metals, and extend their scopes and potentials in a fundamental way for economic efficiency and stability of single‐atom metals. Single‐atom Au modification of molybdenum disulfide quantum dots (MoS2 QDs) will induce a new defect energy level of Au in the forbidden band that can trap excess electrons in n‐type MoS2, which increases the radiative recombination probability of conduction band electrons with valence band holes of MoS2. Thus, 4‐fold enhanced fluorescence efficiency of MoS2 QDs is achieved through single‐atom Au modification.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202207300