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Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect

2D materials are considered for applications that require strong light-matter interaction because of the apparently giant oscillator strength of the exciton transitions in the absorbance spectrum. Nevertheless, the effective oscillator strengths of these transitions have been scarcely reported, nor...

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Autores principales: Geiregat, Pieter, Rodá, Carmelita, Tanghe, Ivo, Singh, Shalini, Di Giacomo, Alessio, Lebrun, Delphine, Grimaldi, Gianluca, Maes, Jorick, Van Thourhout, Dries, Moreels, Iwan, Houtepen, Arjan J., Hens, Zeger
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8165098/
https://www.ncbi.nlm.nih.gov/pubmed/34054127
http://dx.doi.org/10.1038/s41377-021-00548-z
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author Geiregat, Pieter
Rodá, Carmelita
Tanghe, Ivo
Singh, Shalini
Di Giacomo, Alessio
Lebrun, Delphine
Grimaldi, Gianluca
Maes, Jorick
Van Thourhout, Dries
Moreels, Iwan
Houtepen, Arjan J.
Hens, Zeger
author_facet Geiregat, Pieter
Rodá, Carmelita
Tanghe, Ivo
Singh, Shalini
Di Giacomo, Alessio
Lebrun, Delphine
Grimaldi, Gianluca
Maes, Jorick
Van Thourhout, Dries
Moreels, Iwan
Houtepen, Arjan J.
Hens, Zeger
author_sort Geiregat, Pieter
collection PubMed
description 2D materials are considered for applications that require strong light-matter interaction because of the apparently giant oscillator strength of the exciton transitions in the absorbance spectrum. Nevertheless, the effective oscillator strengths of these transitions have been scarcely reported, nor is there a consistent interpretation of the obtained values. Here, we analyse the transition dipole moment and the ensuing oscillator strength of the exciton transition in 2D CdSe nanoplatelets by means of the optically induced Stark effect (OSE). Intriguingly, we find that the exciton absorption line reacts to a high intensity optical field as a transition with an oscillator strength F(Stark) that is 50 times smaller than expected based on the linear absorption coefficient. We propose that the pronounced exciton absorption line should be seen as the sum of multiple, low oscillator strength transitions, rather than a single high oscillator strength one, a feat we assign to strong exciton center-of-mass localization. Within the quantum mechanical description of excitons, this 50-fold difference between both oscillator strengths corresponds to the ratio between the coherence area of the exciton’s center of mass and the total area, which yields a coherence area of a mere 6.1 nm(2). Since we find that the coherence area increases with reducing temperature, we conclude that thermal effects, related to lattice vibrations, contribute to exciton localization. In further support of this localization model, we show that F(Stark) is independent of the nanoplatelet area, correctly predicts the radiative lifetime, and lines up for strongly confined quantum dot systems. [Image: see text]
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spelling pubmed-81650982021-06-15 Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect Geiregat, Pieter Rodá, Carmelita Tanghe, Ivo Singh, Shalini Di Giacomo, Alessio Lebrun, Delphine Grimaldi, Gianluca Maes, Jorick Van Thourhout, Dries Moreels, Iwan Houtepen, Arjan J. Hens, Zeger Light Sci Appl Article 2D materials are considered for applications that require strong light-matter interaction because of the apparently giant oscillator strength of the exciton transitions in the absorbance spectrum. Nevertheless, the effective oscillator strengths of these transitions have been scarcely reported, nor is there a consistent interpretation of the obtained values. Here, we analyse the transition dipole moment and the ensuing oscillator strength of the exciton transition in 2D CdSe nanoplatelets by means of the optically induced Stark effect (OSE). Intriguingly, we find that the exciton absorption line reacts to a high intensity optical field as a transition with an oscillator strength F(Stark) that is 50 times smaller than expected based on the linear absorption coefficient. We propose that the pronounced exciton absorption line should be seen as the sum of multiple, low oscillator strength transitions, rather than a single high oscillator strength one, a feat we assign to strong exciton center-of-mass localization. Within the quantum mechanical description of excitons, this 50-fold difference between both oscillator strengths corresponds to the ratio between the coherence area of the exciton’s center of mass and the total area, which yields a coherence area of a mere 6.1 nm(2). Since we find that the coherence area increases with reducing temperature, we conclude that thermal effects, related to lattice vibrations, contribute to exciton localization. In further support of this localization model, we show that F(Stark) is independent of the nanoplatelet area, correctly predicts the radiative lifetime, and lines up for strongly confined quantum dot systems. [Image: see text] Nature Publishing Group UK 2021-05-31 /pmc/articles/PMC8165098/ /pubmed/34054127 http://dx.doi.org/10.1038/s41377-021-00548-z Text en © The Author(s) 2021 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Geiregat, Pieter
Rodá, Carmelita
Tanghe, Ivo
Singh, Shalini
Di Giacomo, Alessio
Lebrun, Delphine
Grimaldi, Gianluca
Maes, Jorick
Van Thourhout, Dries
Moreels, Iwan
Houtepen, Arjan J.
Hens, Zeger
Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect
title Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect
title_full Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect
title_fullStr Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect
title_full_unstemmed Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect
title_short Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect
title_sort localization-limited exciton oscillator strength in colloidal cdse nanoplatelets revealed by the optically induced stark effect
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8165098/
https://www.ncbi.nlm.nih.gov/pubmed/34054127
http://dx.doi.org/10.1038/s41377-021-00548-z
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