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Direct Visualization and Determination of the Multiple Exciton Generation Rate

[Image: see text] Multiple exciton generation (MEG) takes place in competition to other hot carrier cooling processes. While the determination of carrier cooling rates is well established, direct information on MEG dynamics has been lacking. Here, we present a methodology to obtain the MEG rate dire...

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Autores principales: Timmerman, Dolf, Matsubara, Eiichi, Gomez, Leyre, Ashida, Masaaki, Gregorkiewicz, Tom, Fujiwara, Yasufumi
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2020
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7469370/
https://www.ncbi.nlm.nih.gov/pubmed/32905445
http://dx.doi.org/10.1021/acsomega.0c02067
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author Timmerman, Dolf
Matsubara, Eiichi
Gomez, Leyre
Ashida, Masaaki
Gregorkiewicz, Tom
Fujiwara, Yasufumi
author_facet Timmerman, Dolf
Matsubara, Eiichi
Gomez, Leyre
Ashida, Masaaki
Gregorkiewicz, Tom
Fujiwara, Yasufumi
author_sort Timmerman, Dolf
collection PubMed
description [Image: see text] Multiple exciton generation (MEG) takes place in competition to other hot carrier cooling processes. While the determination of carrier cooling rates is well established, direct information on MEG dynamics has been lacking. Here, we present a methodology to obtain the MEG rate directly in the initial ultrafast transient absorption dynamics. This method is most effective to systems with slow carrier cooling rates. Perovskite quantum dots exhibit this property and are used to illustrate this approach. They show a delayed carrier concentration buildup following an excitation pulse above the MEG threshold energy, which is accompanied by a faster carrier relaxation, providing a direct evidence of the MEG process. Numerical modeling within a simple framework of two competing cooling mechanisms allows us to extract the MEG rate and carrier energy cooling rates for this material. The presented methodology could provide new insights in carrier generation physics and valuable information for MEG investigations.
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spelling pubmed-74693702020-09-04 Direct Visualization and Determination of the Multiple Exciton Generation Rate Timmerman, Dolf Matsubara, Eiichi Gomez, Leyre Ashida, Masaaki Gregorkiewicz, Tom Fujiwara, Yasufumi ACS Omega [Image: see text] Multiple exciton generation (MEG) takes place in competition to other hot carrier cooling processes. While the determination of carrier cooling rates is well established, direct information on MEG dynamics has been lacking. Here, we present a methodology to obtain the MEG rate directly in the initial ultrafast transient absorption dynamics. This method is most effective to systems with slow carrier cooling rates. Perovskite quantum dots exhibit this property and are used to illustrate this approach. They show a delayed carrier concentration buildup following an excitation pulse above the MEG threshold energy, which is accompanied by a faster carrier relaxation, providing a direct evidence of the MEG process. Numerical modeling within a simple framework of two competing cooling mechanisms allows us to extract the MEG rate and carrier energy cooling rates for this material. The presented methodology could provide new insights in carrier generation physics and valuable information for MEG investigations. American Chemical Society 2020-08-19 /pmc/articles/PMC7469370/ /pubmed/32905445 http://dx.doi.org/10.1021/acsomega.0c02067 Text en Copyright © 2020 American Chemical Society This is an open access article published under an ACS AuthorChoice License (http://pubs.acs.org/page/policy/authorchoice_termsofuse.html) , which permits copying and redistribution of the article or any adaptations for non-commercial purposes.
spellingShingle Timmerman, Dolf
Matsubara, Eiichi
Gomez, Leyre
Ashida, Masaaki
Gregorkiewicz, Tom
Fujiwara, Yasufumi
Direct Visualization and Determination of the Multiple Exciton Generation Rate
title Direct Visualization and Determination of the Multiple Exciton Generation Rate
title_full Direct Visualization and Determination of the Multiple Exciton Generation Rate
title_fullStr Direct Visualization and Determination of the Multiple Exciton Generation Rate
title_full_unstemmed Direct Visualization and Determination of the Multiple Exciton Generation Rate
title_short Direct Visualization and Determination of the Multiple Exciton Generation Rate
title_sort direct visualization and determination of the multiple exciton generation rate
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7469370/
https://www.ncbi.nlm.nih.gov/pubmed/32905445
http://dx.doi.org/10.1021/acsomega.0c02067
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