Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor

Transport of excitons in organic materials can be enhanced through polariton formation when the interaction strength between these excitons and the confined light modes of an optical resonator exceeds their decay rates. While the polariton lifetime is determined by the Q(uality)-factor of the optica...

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Detalhes bibliográficos
Autores: Tichauer, Ruth Elena, Sokolovskii, Ilia, Groenhof, Gerrit
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:10486/713436
Acesso em linha:http://hdl.handle.net/10486/713436
https://dx.doi.org/10.1002/advs.202302650
Access Level:acceso abierto
Palavra-chave:Fabry–Pérot cavity
molecular dynamics
polariton
strong light–matter coupling
excitation energy transfer
Física
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spelling Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factorTichauer, Ruth ElenaSokolovskii, IliaGroenhof, GerritFabry–Pérot cavitymolecular dynamicspolaritonstrong light–matter couplingexcitation energy transferFísicaTransport of excitons in organic materials can be enhanced through polariton formation when the interaction strength between these excitons and the confined light modes of an optical resonator exceeds their decay rates. While the polariton lifetime is determined by the Q(uality)-factor of the optical resonator, the polariton group velocity is not. Instead, the latter is solely determined by the polariton dispersion. Yet, experiments suggest that the Q-factor also controls the polariton propagation velocity. To understand this observation, the authors perform molecular dynamics simulations of Rhodamine chromophores strongly coupled to Fabry–Pérot cavities with various Q-factors. The results suggest that propagation in the aforementioned experiments is initially dominated by ballistic motion of upper polariton states at their group velocities, which leads to a rapid expansion of the wavepacket. Cavity decay in combination with non-adiabatic population transfer into dark states, rapidly depletes these bright states, causing the wavepacket to contract. However, because population transfer is reversible, propagation continues, but as a diffusion process, at lower velocity. By controlling the lifetime of bright states, the Q-factor determines the duration of the ballistic phase and the diffusion coefficient in the diffusive regime. Thus, polariton propagation in organic microcavities can be effectively tuned through the Q-factorThis work was supported by the Academy of Finland (Grant 323996), the European Research Council (Grant No. ERC-2016-StG-714870 to Johannes Feist), and by the Spanish Ministry for Science, Innovation, Universities-Agencia Estatal de Investigación (AEI) through Grants (PID2021-125894NB-I00 and CEX2018-000805-M (through the María de Maeztu program for Units of Excellence in Research and Development)John Wiley and Sons IncDepartamento de Física Teórica de la Materia CondensadaFacultad de Ciencias20232023-11-24research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/713436https://dx.doi.org/10.1002/advs.202302650reponame: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:10486/7134362026-06-23T12:46:27Z
dc.title.none.fl_str_mv Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor
title Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor
spellingShingle Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor
Tichauer, Ruth Elena
Fabry–Pérot cavity
molecular dynamics
polariton
strong light–matter coupling
excitation energy transfer
Física
title_short Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor
title_full Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor
title_fullStr Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor
title_full_unstemmed Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor
title_sort Tuning the Coherent Propagation of Organic Exciton-Polaritons through the Cavity Q-factor
dc.creator.none.fl_str_mv Tichauer, Ruth Elena
Sokolovskii, Ilia
Groenhof, Gerrit
author Tichauer, Ruth Elena
author_facet Tichauer, Ruth Elena
Sokolovskii, Ilia
Groenhof, Gerrit
author_role author
author2 Sokolovskii, Ilia
Groenhof, Gerrit
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 Fabry–Pérot cavity
molecular dynamics
polariton
strong light–matter coupling
excitation energy transfer
Física
topic Fabry–Pérot cavity
molecular dynamics
polariton
strong light–matter coupling
excitation energy transfer
Física
description Transport of excitons in organic materials can be enhanced through polariton formation when the interaction strength between these excitons and the confined light modes of an optical resonator exceeds their decay rates. While the polariton lifetime is determined by the Q(uality)-factor of the optical resonator, the polariton group velocity is not. Instead, the latter is solely determined by the polariton dispersion. Yet, experiments suggest that the Q-factor also controls the polariton propagation velocity. To understand this observation, the authors perform molecular dynamics simulations of Rhodamine chromophores strongly coupled to Fabry–Pérot cavities with various Q-factors. The results suggest that propagation in the aforementioned experiments is initially dominated by ballistic motion of upper polariton states at their group velocities, which leads to a rapid expansion of the wavepacket. Cavity decay in combination with non-adiabatic population transfer into dark states, rapidly depletes these bright states, causing the wavepacket to contract. However, because population transfer is reversible, propagation continues, but as a diffusion process, at lower velocity. By controlling the lifetime of bright states, the Q-factor determines the duration of the ballistic phase and the diffusion coefficient in the diffusive regime. Thus, polariton propagation in organic microcavities can be effectively tuned through the Q-factor
publishDate 2023
dc.date.none.fl_str_mv 2023
2023-11-24
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/10486/713436
https://dx.doi.org/10.1002/advs.202302650
url http://hdl.handle.net/10486/713436
https://dx.doi.org/10.1002/advs.202302650
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 John Wiley and Sons Inc
publisher.none.fl_str_mv John Wiley and Sons Inc
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
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score 15.812429

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