Unusual Spectral Diffusion of Single CuInS2 Quantum Dots Sheds Light on the Mechanism of Radiative Decay

S.O.M. Hinterding; M.J.J. Mangnus; P. Tim Prins; H.J. Jöbsis; S. Busatto; D.A.M. Vanmaekelbergh; C. de Mello-Donega; F.T. Rabouw

doi:10.1021/acs.nanolett.0c04239

Unusual Spectral Diffusion of Single CuInS2 Quantum Dots Sheds Light on the Mechanism of Radiative Decay

S.O.M. Hinterding, M.J.J. Mangnus, P. Tim Prins, H.J. Jöbsis, S. Busatto, D.A.M. Vanmaekelbergh, C. de Mello-Donega, F.T. Rabouw

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

The luminescence of CuInS2 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. SingleQD experiments could help settle this debate, but studies by
different groups have yielded conflicting results. Here, we study the
photophysics of single core-only CuInS2 and core/shell CuInS2/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
CuInS2-based QDs is qualitatively and quantitatively different from
CdSe-based QDs. The differences reflect the dipole moment of the
CuInS2 excited state and hole localization on a preferred site in the
QD. Our results unravel the highly dynamic photophysics of CuInS2
QDs and highlight the power of the analysis of single-QD property fluctuations.

Original language	English
Pages (from-to)	658-665
Number of pages	8
Journal	Nano Letters
Volume	21
Issue number	1
DOIs	https://doi.org/10.1021/acs.nanolett.0c04239
Publication status	Published - 13 Jan 2021

Bibliographical note

Funding Information:
This work was supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture, and Science of the government of The Netherlands. P.T.P., H.J.J., D.V., and C.M.D. acknowledge support from The Netherlands Organization for Scientific Research (NWO, Grant 14614 “Q-Lumicon”). F.T.R. acknowledges financial support from The Netherlands Organization for Scientific Research NWO (VENI Grant 722.017.002). The authors thank the SOLEIL synchrotron, Saint-Aubin, France, for granting beamtime under proposal number 20181211. Javier Pérez is thanked for support during the synchrotron experiments.

Publisher Copyright:
©

Keywords

CuInS
Quantum dots
single-quantum-dot spectroscopy
spectral diffusion

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Cite this

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title = "Unusual Spectral Diffusion of Single CuInS2 Quantum Dots Sheds Light on the Mechanism of Radiative Decay",

abstract = "The luminescence of CuInS2 quantum dots (QDs) isslower and spectrally broader than that of many other types of QDs.The origin of this anomalous behavior is still under debate. SingleQD experiments could help settle this debate, but studies bydifferent groups have yielded conflicting results. Here, we study thephotophysics of single core-only CuInS2 and core/shell CuInS2/CdSQDs. Both types of single QDs exhibit broad PL spectra withfluctuating peak position and single-exponential photoluminescencedecay with a slow but fluctuating lifetime. Spectral diffusion ofCuInS2-based QDs is qualitatively and quantitatively different fromCdSe-based QDs. The differences reflect the dipole moment of theCuInS2 excited state and hole localization on a preferred site in theQD. Our results unravel the highly dynamic photophysics of CuInS2QDs and highlight the power of the analysis of single-QD property fluctuations.",

keywords = "CuInS, Quantum dots, single-quantum-dot spectroscopy, spectral diffusion",

author = "S.O.M. Hinterding and M.J.J. Mangnus and Prins, {P. Tim} and H.J. J{\"o}bsis and S. Busatto and D.A.M. Vanmaekelbergh and {de Mello-Donega}, C. and F.T. Rabouw",

note = "Funding Information: This work was supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture, and Science of the government of The Netherlands. P.T.P., H.J.J., D.V., and C.M.D. acknowledge support from The Netherlands Organization for Scientific Research (NWO, Grant 14614 “Q-Lumicon”). F.T.R. acknowledges financial support from The Netherlands Organization for Scientific Research NWO (VENI Grant 722.017.002). The authors thank the SOLEIL synchrotron, Saint-Aubin, France, for granting beamtime under proposal number 20181211. Javier P{\'e}rez is thanked for support during the synchrotron experiments. Publisher Copyright: {\textcopyright}",

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doi = "10.1021/acs.nanolett.0c04239",

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AU - Hinterding, S.O.M.

AU - Mangnus, M.J.J.

AU - Prins, P. Tim

AU - Jöbsis, H.J.

AU - Busatto, S.

AU - Vanmaekelbergh, D.A.M.

AU - de Mello-Donega, C.

AU - Rabouw, F.T.

N1 - Funding Information: This work was supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture, and Science of the government of The Netherlands. P.T.P., H.J.J., D.V., and C.M.D. acknowledge support from The Netherlands Organization for Scientific Research (NWO, Grant 14614 “Q-Lumicon”). F.T.R. acknowledges financial support from The Netherlands Organization for Scientific Research NWO (VENI Grant 722.017.002). The authors thank the SOLEIL synchrotron, Saint-Aubin, France, for granting beamtime under proposal number 20181211. Javier Pérez is thanked for support during the synchrotron experiments. Publisher Copyright: ©

PY - 2021/1/13

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N2 - The luminescence of CuInS2 quantum dots (QDs) isslower and spectrally broader than that of many other types of QDs.The origin of this anomalous behavior is still under debate. SingleQD experiments could help settle this debate, but studies bydifferent groups have yielded conflicting results. Here, we study thephotophysics of single core-only CuInS2 and core/shell CuInS2/CdSQDs. Both types of single QDs exhibit broad PL spectra withfluctuating peak position and single-exponential photoluminescencedecay with a slow but fluctuating lifetime. Spectral diffusion ofCuInS2-based QDs is qualitatively and quantitatively different fromCdSe-based QDs. The differences reflect the dipole moment of theCuInS2 excited state and hole localization on a preferred site in theQD. Our results unravel the highly dynamic photophysics of CuInS2QDs and highlight the power of the analysis of single-QD property fluctuations.

AB - The luminescence of CuInS2 quantum dots (QDs) isslower and spectrally broader than that of many other types of QDs.The origin of this anomalous behavior is still under debate. SingleQD experiments could help settle this debate, but studies bydifferent groups have yielded conflicting results. Here, we study thephotophysics of single core-only CuInS2 and core/shell CuInS2/CdSQDs. Both types of single QDs exhibit broad PL spectra withfluctuating peak position and single-exponential photoluminescencedecay with a slow but fluctuating lifetime. Spectral diffusion ofCuInS2-based QDs is qualitatively and quantitatively different fromCdSe-based QDs. The differences reflect the dipole moment of theCuInS2 excited state and hole localization on a preferred site in theQD. Our results unravel the highly dynamic photophysics of CuInS2QDs and highlight the power of the analysis of single-QD property fluctuations.

KW - CuInS

KW - Quantum dots

KW - single-quantum-dot spectroscopy

KW - spectral diffusion

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U2 - 10.1021/acs.nanolett.0c04239

DO - 10.1021/acs.nanolett.0c04239

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JO - Nano Letters

JF - Nano Letters

IS - 1

ER -

Unusual Spectral Diffusion of Single CuInS2 Quantum Dots Sheds Light on the Mechanism of Radiative Decay

Abstract

Bibliographical note

Keywords

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