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: | ; ; ; ; |
|---|---|
| Tipo de documento: | Artículo |
| Fecha de publicación: | 2025 |
| País: | España |
| Institución: | Universidad Autónoma de Madrid |
| Repositorio: | Biblos-e Archivo. Repositorio Institucional de la UAM |
| Lenguaje: | 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 |
| Nivel de acceso: | Acceso abierto |
| Palabra clave: | Cavities energy molecules polaritons polarization Física |
| _version_ | 1878742383175139328 |
|---|---|
| author | Bhuyan, Rahul |
| author2 | Lednev, Maksim Schäfer, Clara Feist, Johannes Maximilian Börjesson, Karl |
| author2_role | author author author author |
| author_browse | Bhuyan, Rahul Börjesson, Karl Feist, Johannes Maximilian Lednev, Maksim Schäfer, Clara |
| author_facet | Bhuyan, Rahul Lednev, Maksim Schäfer, Clara Feist, Johannes Maximilian Börjesson, Karl |
| author_role | author |
| collection | Biblos-e Archivo. Repositorio Institucional de la UAM |
| 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 |
| eu_rights_str_mv | openAccess |
| format | article |
| id | ES_f4e9e1bbd239dca720fca9ce431a7def |
| identifier_str_mv | 40524642 |
| institution | Universidad Autónoma de Madrid |
| instname_str | Universidad Autónoma de Madrid |
| language | eng |
| network_acronym_str | ES |
| network_name_str | España |
| oai_identifier_str | oai:repositorio.uam.es:10486/752760 |
| publishDate | 2025 |
| publishDateSort | 2025 |
| publisher | American Chemical Society |
| publisherStr | American Chemical Society |
| reponame_str | Biblos-e Archivo. Repositorio Institucional de la UAM |
| spelling | Quantitative Modeling of Polaritonic Emission Using the Source Term Method Bhuyan, Rahul Lednev, Maksim Schäfer, Clara Feist, Johannes Maximilian Börjesson, Karl Cavities energy molecules polaritons polarization Física 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 K.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 Society https://hdl.handle.net/10486/752760 https://dx.doi.org/10.1021/acs.jpclett.5c01213 40524642 |
| spellingShingle | Quantitative Modeling of Polaritonic Emission Using the Source Term Method Bhuyan, Rahul Cavities energy molecules polaritons polarization Física |
| title | 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_short | Quantitative Modeling of Polaritonic Emission Using the Source Term Method |
| title_sort | Quantitative Modeling of Polaritonic Emission Using the Source Term Method |
| topic | Cavities energy molecules polaritons polarization Física |
| topic_facet | Cavities energy molecules polaritons polarization Física |
| url | https://hdl.handle.net/10486/752760 https://dx.doi.org/10.1021/acs.jpclett.5c01213 |