Molecular polaritonics in dense mesoscopic disordered ensembles
Christian Sommer,
Michael Reitz,
Francesca Mineo,
Claudiu Genes
Physical Review Research
3
(3)
033141
(2021)
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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 (Förster 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.
Excitation transport with collective radiative decay
We investigate a one-dimensional quantum emitter chain where transport of excitations and correlations takes place via nearest neighbor, dipole-dipole interactions. In the presence of collective radiative emission, we show that a phase imprinting wavepacket initialization procedure can lead to subradiant transport and can preserve quantum correlations. In the context of cavity mediated transport, where emitters are coupled to a common delocalized optical mode, we analyze the effect of frequency disorder and nonidentical photon-emitter couplings on excitation transport.
