Quantitative Modeling of Polaritonic Emission Using the Source Term Method
Strong exciton-photon coupling leads to the formation of hybrid states, polaritons, with properties different from those of their constituents, making it a valuable tool for modifying the physical and chemical properties of organic and inorganic materials. Despite its potential, the field lacks a fu...
| Autores: | , , , , |
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| Tipo de recurso: | artículo |
| Fecha de publicación: | 2025 |
| País: | España |
| Institución: | Universidad Autónoma de Madrid |
| Repositorio: | Biblos-e Archivo. Repositorio Institucional de la UAM |
| Idioma: | inglés |
| OAI Identifier: | oai:repositorio.uam.es:10486/752760 |
| Acceso en línea: | https://hdl.handle.net/10486/752760 https://dx.doi.org/10.1021/acs.jpclett.5c01213 |
| Access Level: | acceso abierto |
| Palabra clave: | Cavities energy molecules polaritons polarization Física |
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Quantitative Modeling of Polaritonic Emission Using the Source Term MethodBhuyan, RahulLednev, MaksimSchäfer, ClaraFeist, Johannes MaximilianBörjesson, KarlCavitiesenergymoleculespolaritonspolarizationFísicaStrong exciton-photon coupling leads to the formation of hybrid states, polaritons, with properties different from those of their constituents, making it a valuable tool for modifying the physical and chemical properties of organic and inorganic materials. Despite its potential, the field lacks a fundamental understanding of the photophysics involved and the ability to model experimental data effectively. In this study, we quantitatively simulate polaritonic emission using the source term method. This model assumes that each molecular dipole in the exciton reservoir emits as it would in free space, into the optical environment formed by the polaritons. To benchmark theory with experiments, a BODIPY derivative containing a suitable amount of steric bulk was synthesized. Neat films of this molecule exhibited close to unperturbed absorption and emission envelopes compared to dilute solution. When placed in an optical cavity, the ultrastrong coupling regime was reached, and a collapse of the polaritonic line width was observed. Such a collapse is an indication of an ideal polariton, and it allowed for the emission in the transverse electric and magnetic polarizations to be spectrally resolved and thus successfully compared to the simulated emission. This work hence describes an effective model that fits experimental data, which is crucial for advancing the field and for optimizing applicationsK.B. gratefully acknowledge financial support from the Knut and Alice Wallenberg Foundation (KAW 2017,0192), the Swedish Research Council (2020-03578), the European Research Council (ERC-2023-COG-101124329; CONTROL) and the Göran Gustafsson foundation. M.L. and J.F. gratefully acknowledge support by the Spanish Ministry of Science and Innovation - Agencia Estatal de Investigación through grants PID2021-125894NB-I00, EUR2023-143478, and CEX2018- 000805-M (through the María de Maeztu program for Units of Excellence in R&D), and PRE2021-098978 (to M.L. with support from ESF+). In addition, this project received funding from the European Union’s Horizon 2020 research and innovation program through Agreement No. 101098813 (SCOLED)American Chemical SocietyDepartamento de Física Teórica de la Materia CondensadaFacultad de CienciasEuropean Research CouncilGobierno de España20252025-06-17research articlehttp://purl.org/coar/resource_type/c_2df8fbb1EVoRhttp://purl.org/coar/version/c_dc82b40f9837b551info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/10486/752760https://dx.doi.org/10.1021/acs.jpclett.5c0121340524642reponame: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:10486/7527602026-06-23T12:46:27Z |
| dc.title.none.fl_str_mv |
Quantitative Modeling of Polaritonic Emission Using the Source Term Method |
| title |
Quantitative Modeling of Polaritonic Emission Using the Source Term Method |
| spellingShingle |
Quantitative Modeling of Polaritonic Emission Using the Source Term Method Bhuyan, Rahul Cavities energy molecules polaritons polarization Física |
| title_short |
Quantitative Modeling of Polaritonic Emission Using the Source Term Method |
| title_full |
Quantitative Modeling of Polaritonic Emission Using the Source Term Method |
| title_fullStr |
Quantitative Modeling of Polaritonic Emission Using the Source Term Method |
| title_full_unstemmed |
Quantitative Modeling of Polaritonic Emission Using the Source Term Method |
| title_sort |
Quantitative Modeling of Polaritonic Emission Using the Source Term Method |
| dc.creator.none.fl_str_mv |
Bhuyan, Rahul Lednev, Maksim Schäfer, Clara Feist, Johannes Maximilian Börjesson, Karl |
| author |
Bhuyan, Rahul |
| author_facet |
Bhuyan, Rahul Lednev, Maksim Schäfer, Clara Feist, Johannes Maximilian Börjesson, Karl |
| author_role |
author |
| author2 |
Lednev, Maksim Schäfer, Clara Feist, Johannes Maximilian Börjesson, Karl |
| author2_role |
author author author author |
| dc.contributor.none.fl_str_mv |
Departamento de Física Teórica de la Materia Condensada Facultad de Ciencias European Research Council Gobierno de España |
| dc.subject.none.fl_str_mv |
Cavities energy molecules polaritons polarization Física |
| topic |
Cavities energy molecules polaritons polarization Física |
| description |
Strong exciton-photon coupling leads to the formation of hybrid states, polaritons, with properties different from those of their constituents, making it a valuable tool for modifying the physical and chemical properties of organic and inorganic materials. Despite its potential, the field lacks a fundamental understanding of the photophysics involved and the ability to model experimental data effectively. In this study, we quantitatively simulate polaritonic emission using the source term method. This model assumes that each molecular dipole in the exciton reservoir emits as it would in free space, into the optical environment formed by the polaritons. To benchmark theory with experiments, a BODIPY derivative containing a suitable amount of steric bulk was synthesized. Neat films of this molecule exhibited close to unperturbed absorption and emission envelopes compared to dilute solution. When placed in an optical cavity, the ultrastrong coupling regime was reached, and a collapse of the polaritonic line width was observed. Such a collapse is an indication of an ideal polariton, and it allowed for the emission in the transverse electric and magnetic polarizations to be spectrally resolved and thus successfully compared to the simulated emission. This work hence describes an effective model that fits experimental data, which is crucial for advancing the field and for optimizing applications |
| publishDate |
2025 |
| dc.date.none.fl_str_mv |
2025 2025-06-17 |
| dc.type.none.fl_str_mv |
research article http://purl.org/coar/resource_type/c_2df8fbb1 EVoR http://purl.org/coar/version/c_dc82b40f9837b551 |
| dc.type.openaire.fl_str_mv |
info:eu-repo/semantics/article |
| format |
article |
| dc.identifier.none.fl_str_mv |
https://hdl.handle.net/10486/752760 https://dx.doi.org/10.1021/acs.jpclett.5c01213 40524642 |
| url |
https://hdl.handle.net/10486/752760 https://dx.doi.org/10.1021/acs.jpclett.5c01213 |
| identifier_str_mv |
40524642 |
| 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/ |
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info:eu-repo/semantics/openAccess |
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open access http://purl.org/coar/access_right/c_abf2 Attribution 4.0 International http://creativecommons.org/licenses/by/4.0/ |
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openAccess |
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application/pdf |
| dc.publisher.none.fl_str_mv |
American Chemical Society |
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American Chemical Society |
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reponame:Biblos-e Archivo. Repositorio Institucional de la UAM instname:Universidad Autónoma de Madrid |
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Universidad Autónoma de Madrid |
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Biblos-e Archivo. Repositorio Institucional de la UAM |
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Biblos-e Archivo. Repositorio Institucional de la UAM |
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