Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime

Strong interactions between excitons and photons lead to the formation of exciton-polaritons, which possess completely different properties compared to their constituents. The polaritons are created by incorporating a material in an optical cavity where the electromagnetic field is tightly confined....

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Detalhes bibliográficos
Autores: Mukherjee, Arpita, Feist, Johannes, Börjesson, Karl
Formato: artículo
Fecha de publicación:2023
País:España
Recursos:Universidad Autónoma de Madrid
Repositorio:Biblos-e Archivo. Repositorio Institucional de la UAM
Idioma:inglés
OAI Identifier:oai:repositorio.uam.es:10486/714416
Acesso em linha:http://hdl.handle.net/10486/714416
https://dx.doi.org/10.1021/jacs.2c11531
Access Level:acceso abierto
Palavra-chave:Strong interactions
excitons
photons
exciton-polaritons
properties
optical cavity
electromagnetic field
polaritonic states
energy transfer
Förster radius
Física
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spelling Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling RegimeMukherjee, ArpitaFeist, JohannesBörjesson, KarlStrong interactionsexcitonsphotonsexciton-polaritonspropertiesoptical cavityelectromagnetic fieldpolaritonic statesenergy transferFörster radiusFísicaStrong interactions between excitons and photons lead to the formation of exciton-polaritons, which possess completely different properties compared to their constituents. The polaritons are created by incorporating a material in an optical cavity where the electromagnetic field is tightly confined. Over the last few years, the relaxation of polaritonic states has been shown to enable a new kind of energy transfer event, which is efficient at length scales substantially larger than the typical Förster radius. However, the importance of such energy transfer depends on the ability of the short-lived polaritonic states to efficiently decay to molecular localized states that can perform a photochemical process, such as charge transfer or triplet states. Here, we investigate quantitatively the interaction between polaritons and triplet states of erythrosine B in the strong coupling regime. We analyze the experimental data, collected mainly employing angle-resolved reflectivity and excitation measurements, using a rate equation model. We show that the rate of intersystem crossing from the polariton to the triplet states depends on the energy alignment of the excited polaritonic states. Furthermore, it is demonstrated that the rate of intersystem crossing can be substantially enhanced in the strong coupling regime to the point where it approaches the rate of the radiative decay of the polariton. In light of the opportunities that transitions from polaritonic to molecular localized states offer within molecular photophysics/chemistry and organic electronics, we hope that the quantitative understanding of such interactions gained from this study will aid in the development of polariton-empowered devicesThe authors gratefully acknowledge financial support from the European Research council (ERC-2017-StG-757733 and ERC-2016-StG-714870) and by the Spanish Ministry for Science, Innovation, and Universities-Agencia Estatal de Investigación through Grants PID2021-125894NB-I00 and CEX2018-000805-M (through the María de Maeztu program for Units of Excellence in R&D)American Chemical SocietyDepartamento de Física Teórica de la Materia CondensadaFacultad de Ciencias20232023-03-08research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/714416https://dx.doi.org/10.1021/jacs.2c11531reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution 4.0 Internationalhttp://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7144162026-06-23T12:46:27Z
dc.title.none.fl_str_mv Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime
title Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime
spellingShingle Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime
Mukherjee, Arpita
Strong interactions
excitons
photons
exciton-polaritons
properties
optical cavity
electromagnetic field
polaritonic states
energy transfer
Förster radius
Física
title_short Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime
title_full Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime
title_fullStr Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime
title_full_unstemmed Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime
title_sort Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime
dc.creator.none.fl_str_mv Mukherjee, Arpita
Feist, Johannes
Börjesson, Karl
author Mukherjee, Arpita
author_facet Mukherjee, Arpita
Feist, Johannes
Börjesson, Karl
author_role author
author2 Feist, Johannes
Börjesson, Karl
author2_role author
author
dc.contributor.none.fl_str_mv Departamento de Física Teórica de la Materia Condensada
Facultad de Ciencias
dc.subject.none.fl_str_mv Strong interactions
excitons
photons
exciton-polaritons
properties
optical cavity
electromagnetic field
polaritonic states
energy transfer
Förster radius
Física
topic Strong interactions
excitons
photons
exciton-polaritons
properties
optical cavity
electromagnetic field
polaritonic states
energy transfer
Förster radius
Física
description Strong interactions between excitons and photons lead to the formation of exciton-polaritons, which possess completely different properties compared to their constituents. The polaritons are created by incorporating a material in an optical cavity where the electromagnetic field is tightly confined. Over the last few years, the relaxation of polaritonic states has been shown to enable a new kind of energy transfer event, which is efficient at length scales substantially larger than the typical Förster radius. However, the importance of such energy transfer depends on the ability of the short-lived polaritonic states to efficiently decay to molecular localized states that can perform a photochemical process, such as charge transfer or triplet states. Here, we investigate quantitatively the interaction between polaritons and triplet states of erythrosine B in the strong coupling regime. We analyze the experimental data, collected mainly employing angle-resolved reflectivity and excitation measurements, using a rate equation model. We show that the rate of intersystem crossing from the polariton to the triplet states depends on the energy alignment of the excited polaritonic states. Furthermore, it is demonstrated that the rate of intersystem crossing can be substantially enhanced in the strong coupling regime to the point where it approaches the rate of the radiative decay of the polariton. In light of the opportunities that transitions from polaritonic to molecular localized states offer within molecular photophysics/chemistry and organic electronics, we hope that the quantitative understanding of such interactions gained from this study will aid in the development of polariton-empowered devices
publishDate 2023
dc.date.none.fl_str_mv 2023
2023-03-08
dc.type.none.fl_str_mv research article
http://purl.org/coar/resource_type/c_2df8fbb1
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10486/714416
https://dx.doi.org/10.1021/jacs.2c11531
url http://hdl.handle.net/10486/714416
https://dx.doi.org/10.1021/jacs.2c11531
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution 4.0 International
http://creativecommons.org/licenses/by/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution 4.0 International
http://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:Biblos-e Archivo. Repositorio Institucional de la UAM
instname:Universidad Autónoma de Madrid
instname_str Universidad Autónoma de Madrid
reponame_str Biblos-e Archivo. Repositorio Institucional de la UAM
collection Biblos-e Archivo. Repositorio Institucional de la UAM
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869420666222018560
score 15,198674

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