Molecular polaritonics in dense mesoscopic disordered ensembles
| Autor: | Claudiu Genes, Francesca Mineo, Michael Reitz, Christian Sommer |
|---|---|
| Rok vydání: | 2021 |
| Předmět: |
Physics
Quantum Physics Mesoscopic physics Condensed Matter - Mesoscale and Nanoscale Physics Cavity quantum electrodynamics FOS: Physical sciences Resonance (particle physics) Molecular physics Vibronic coupling Dark state Mesoscale and Nanoscale Physics (cond-mat.mes-hall) Dissipative system Vibrational energy relaxation Polaritonics Quantum Physics (quant-ph) |
| Zdroj: | Physical Review Research |
| ISSN: | 2643-1564 |
| DOI: | 10.1103/physrevresearch.3.033141 |
| Popis: | We study the dependence of the vacuum Rabi splitting (VRS) on frequency disorder, vibrations, near-field effects and density in molecular polaritonics. In the mesoscopic limit, static frequency disorder alone can already introduce a loss mechanism from polaritonic states into a dark state reservoir, which we quantitatively describe, providing an analytical scaling of the VRS with the level of disorder. Disorder additionally can split a molecular ensemble into donor-type and acceptor-type molecules and the combination of vibronic coupling, dipole-dipole interactions and vibrational relaxation induces an incoherent FRET (F\"{o}rster resonance energy transfer) migration of excitations within the collective molecular state. This is equivalent to a dissipative disorder and has the effect of saturating and even reducing the VRS in the mesoscopic, high-density limit. Overall, this analysis allows to quantify the crucial role played by dark states in cavity quantum electrodynamics with mesoscopic, disordered ensembles. |
| Databáze: | OpenAIRE |
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