Enhanced Excitation Energy Transfer under Strong Light-Matter Coupling: Insights from Multi-Scale Molecular Dynamics Simulations
Fuente:
arXiv
Saved in:
| Main Authors: | , , , , |
|---|---|
| Format: | Preprint |
| Published: |
2022
|
| Subjects: | |
| Online Access: | |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866913270642769920 |
|---|---|
| author | Sokolovskii, Ilia Tichauer, Ruth H. Morozov, Dmitry Feist, Johannes Groenhof, Gerrit |
| author_facet | Sokolovskii, Ilia Tichauer, Ruth H. Morozov, Dmitry Feist, Johannes Groenhof, Gerrit |
| contents | Exciton transport can be enhanced in the strong coupling regime where excitons hybridise with confined light modes to form polaritons. Because polaritons have group velocity, their propagation should be ballistic and long-ranged. However, experiments indicate that organic polaritons propagate in a diffusive manner and more slowly than their group velocity. Here, we resolve this controversy by means of molecular dynamics simulations of Rhodamine molecules in a Fabry-Pérot cavity. Our results suggest that polariton propagation is limited by the cavity lifetime and appears diffusive due to reversible population transfers between polaritonic states that propagate ballistically at their group velocity, and dark states that are stationary. Furthermore, because long-lived dark states transiently trap the excitation, propagation is observed on timescales beyond the intrinsic polariton lifetime. These insights not only help to better understand and interpret experimental observations, but also pave the way towards rational design of molecule-cavity systems for coherent exciton transport. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2209_07309 |
| institution | arXiv |
| publishDate | 2022 |
| record_format | arxiv |
| spellingShingle | Enhanced Excitation Energy Transfer under Strong Light-Matter Coupling: Insights from Multi-Scale Molecular Dynamics Simulations Sokolovskii, Ilia Tichauer, Ruth H. Morozov, Dmitry Feist, Johannes Groenhof, Gerrit Chemical Physics Exciton transport can be enhanced in the strong coupling regime where excitons hybridise with confined light modes to form polaritons. Because polaritons have group velocity, their propagation should be ballistic and long-ranged. However, experiments indicate that organic polaritons propagate in a diffusive manner and more slowly than their group velocity. Here, we resolve this controversy by means of molecular dynamics simulations of Rhodamine molecules in a Fabry-Pérot cavity. Our results suggest that polariton propagation is limited by the cavity lifetime and appears diffusive due to reversible population transfers between polaritonic states that propagate ballistically at their group velocity, and dark states that are stationary. Furthermore, because long-lived dark states transiently trap the excitation, propagation is observed on timescales beyond the intrinsic polariton lifetime. These insights not only help to better understand and interpret experimental observations, but also pave the way towards rational design of molecule-cavity systems for coherent exciton transport. |
| title | Enhanced Excitation Energy Transfer under Strong Light-Matter Coupling: Insights from Multi-Scale Molecular Dynamics Simulations |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2209.07309 |