Molecular polaritonics in dense mesoscopic disordered ensembles

Sommer C, Reitz M, Mineo F, Genes C (2021)

Publication Type: Journal article

Publication year: 2021

Journal

Physical Review Research American Physical Society

Book Volume: 3

Journal Issue: 3

DOI: 10.1103/PhysRevResearch.3.033141

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 (Forster 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.

Additional Organisation(s)

Sonderforschungsbereich/Transregio 306/1: Quantenkooperativität von Licht und Materie - QuCoLiMa

Related research project(s)

Cooperative effects in coupled quantum emitter systems (D01) TRR 306: Quantenkooperativität von Licht und Materie – QuCoLiMa Jan. 1, 2021 - Dec. 31, 2024

Involved external institutions

Max-Planck-Institut für die Physik des Lichts (MPL) / Max Planck Institute for the Science of Light DE Germany (DE)

How to cite

APA:

Sommer, C., Reitz, M., Mineo, F., & Genes, C. (2021). Molecular polaritonics in dense mesoscopic disordered ensembles. Physical Review Research, 3(3). https://doi.org/10.1103/PhysRevResearch.3.033141

MLA:

Sommer, C., et al. "Molecular polaritonics in dense mesoscopic disordered ensembles." Physical Review Research 3.3 (2021).

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