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Unusual Spectral Diffusion of Single CuInS2 Quantum Dots Sheds Light on the Mechanism of Radiative Decay
Author(s) -
Stijn O. M. Hinterding,
Mark J. J. Mangnus,
P. Tim Prins,
Huygen J. Jöbsis,
Serena Busatto,
Daniël Vanmaekelbergh,
Celso de Mello Donegá,
Freddy T. Rabouw
Publication year - 2021
Publication title -
nano letters
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 4.853
H-Index - 488
eISSN - 1530-6992
pISSN - 1530-6984
DOI - 10.1021/acs.nanolett.0c04239
Subject(s) - quantum dot , photoluminescence , luminescence , excited state , diffusion , dipole , molecular physics , chemical physics , materials science , radiative transfer , core (optical fiber) , spectral line , chemistry , optoelectronics , atomic physics , physics , optics , organic chemistry , composite material , astronomy , thermodynamics
The luminescence of CuInS 2 quantum dots (QDs) is slower and spectrally broader than that of many other types of QDs. The origin of this anomalous behavior is still under debate. Single-QD experiments could help settle this debate, but studies by different groups have yielded conflicting results. Here, we study the photophysics of single core-only CuInS 2 and core/shell CuInS 2 /CdS QDs. Both types of single QDs exhibit broad PL spectra with fluctuating peak position and single-exponential photoluminescence decay with a slow but fluctuating lifetime. Spectral diffusion of CuInS 2 -based QDs is qualitatively and quantitatively different from CdSe-based QDs. The differences reflect the dipole moment of the CuInS 2 excited state and hole localization on a preferred site in the QD. Our results unravel the highly dynamic photophysics of CuInS 2 QDs and highlight the power of the analysis of single-QD property fluctuations.

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