Tuning the Coherent Propagation of Organic Exciton‐Polaritons through the Cavity Q‐factor
Abstract 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 t...
| Main Authors: | , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Wiley
2023-11-01
|
| Series: | Advanced Science |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/advs.202302650 |
| _version_ | 1797465025215987712 |
|---|---|
| author | Ruth H. Tichauer Ilia Sokolovskii Gerrit Groenhof |
| author_facet | Ruth H. Tichauer Ilia Sokolovskii Gerrit Groenhof |
| author_sort | Ruth H. Tichauer |
| collection | DOAJ |
| description | Abstract 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. |
| first_indexed | 2024-03-09T18:16:36Z |
| format | Article |
| id | doaj.art-56f68ac9603d4e98ba318da1d20d1438 |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-03-09T18:16:36Z |
| publishDate | 2023-11-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-56f68ac9603d4e98ba318da1d20d14382023-11-24T08:40:29ZengWileyAdvanced Science2198-38442023-11-011033n/an/a10.1002/advs.202302650Tuning the Coherent Propagation of Organic Exciton‐Polaritons through the Cavity Q‐factorRuth H. Tichauer0Ilia Sokolovskii1Gerrit Groenhof2Departamento de Física Teórica de la Materia Condensada and Condensed Matter Physics Center (IFIMAC) Universidad Autónoma de Madrid Madrid E‐28049 SpainNanoscience Center and Department of Chemistry University of Jyväskylä P.O. Box 35, 40014 Jyväskylä FinlandNanoscience Center and Department of Chemistry University of Jyväskylä P.O. Box 35, 40014 Jyväskylä FinlandAbstract 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.https://doi.org/10.1002/advs.202302650excitation energy transferFabry–Pérot cavitymolecular dynamicspolaritonstrong light–matter coupling |
| spellingShingle | Ruth H. Tichauer Ilia Sokolovskii Gerrit Groenhof Tuning the Coherent Propagation of Organic Exciton‐Polaritons through the Cavity Q‐factor Advanced Science excitation energy transfer Fabry–Pérot cavity molecular dynamics polariton strong light–matter coupling |
| title | 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_short | 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 |
| topic | excitation energy transfer Fabry–Pérot cavity molecular dynamics polariton strong light–matter coupling |
| url | https://doi.org/10.1002/advs.202302650 |
| work_keys_str_mv | AT ruthhtichauer tuningthecoherentpropagationoforganicexcitonpolaritonsthroughthecavityqfactor AT iliasokolovskii tuningthecoherentpropagationoforganicexcitonpolaritonsthroughthecavityqfactor AT gerritgroenhof tuningthecoherentpropagationoforganicexcitonpolaritonsthroughthecavityqfactor |