Molecular polaritonics in dense mesoscopic disordered ensembles
- URL: http://arxiv.org/abs/2010.07155v2
- Date: Fri, 20 Aug 2021 14:13:13 GMT
- Title: Molecular polaritonics in dense mesoscopic disordered ensembles
- Authors: Christian Sommer, Michael Reitz, Francesca Mineo and Claudiu Genes
- Abstract summary: We study the dependence of the vacuum Rabi splitting (VRS) on frequency disorder, vibrations, near-field effects and density in molecular polaritonics.
- Score: 0.3058685580689604
- License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
- 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 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.
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