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Molecular polaritonics in dense mesoscopic disordered ensembles

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Sommer,  Christian
Genes Research Group, Research Groups, Max Planck Institute for the Science of Light, Max Planck Society;

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Reitz,  Michael
Genes Research Group, Research Groups, Max Planck Institute for the Science of Light, Max Planck Society;
International Max Planck Research School, Max Planck Institute for the Science of Light, Max Planck Society;

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Mineo,  Francesca
International Max Planck Research School, Max Planck Institute for the Science of Light, Max Planck Society;
Genes Research Group, Research Groups, Max Planck Institute for the Science of Light, Max Planck Society;

/persons/resource/persons216190

Genes,  Claudiu
Genes Research Group, Research Groups, Max Planck Institute for the Science of Light, Max Planck Society;

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Citation

Sommer, C., Reitz, M., Mineo, F., & Genes, C. (2020). Molecular polaritonics in dense mesoscopic disordered ensembles. arXiv: 2010.07155.


Cite as: http://hdl.handle.net/21.11116/0000-0007-4258-C
Abstract
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 introduces a loss mechanism from polaritonic states into a dark state reservoir, which we quantitatively describe, providing an analytical scaling of the VRS on the level of disorder. The combination of disorder, vibronic coupling, dipole-dipole interactions and vibrational relaxation induces an incoherent FRET (Forster resonance energy transfer) migration of excitations from donor-type to acceptor-type molecules 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.