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Thermalization rate of polaritons in strongly-coupled molecular systems

Autor(en)
Evgeny A. Tereshchenkov, Ivan V. Panyukov, Mikhail Misko, Vladislav Y. Shishkov, Evgeny S. Andrianov, Anton V. Zasedatelev
Abstrakt

Polariton thermalization is a key process in achieving light–matter Bose–Einstein condensation, spanning from solid-state semiconductor microcavities at cryogenic temperatures to surface plasmon nanocavities with molecules at room temperature. Originated from the matter component of polariton states, the microscopic mechanisms of thermalization are closely tied to specific material properties. In this work, we investigate polariton thermalization in strongly-coupled molecular systems. We develop a microscopic theory addressing polariton thermalization through electron-phonon interactions (known as exciton-vibration coupling) with low-energy molecular vibrations. This theory presents a simple analytical method to calculate the temperature-dependent polariton thermalization rate, utilizing experimentally accessible spectral properties of bare molecules, such as the Stokes shift and temperature-dependent linewidth of photoluminescence, in conjunction with well-known parameters of optical cavities. Our findings demonstrate qualitative agreement with recent experimental reports of nonequilibrium polariton condensation in both ground and excited states, and explain the thermalization bottleneck effect observed at low temperatures. This study showcases the significance of vibrational degrees of freedom in polariton condensation and offers practical guidance for future experiments, including the selection of suitable material systems and cavity designs.

Organisation(en)
Quantenoptik, Quantennanophysik und Quanteninformation
Externe Organisation(en)
Dukhov Research Institute of Automatics (VNIIA), Russian Academy of Sciences, Moscow Institute of Physics and Technology
Journal
Nanophotonics
Band
13
Seiten
2635–2649
Anzahl der Seiten
15
ISSN
2192-8614
DOI
https://doi.org/10.48550/arXiv.2311.09896
Publikationsdatum
03-2024
Peer-reviewed
Ja
ÖFOS 2012
103025 Quantenmechanik, 103021 Optik
Schlagwörter
ASJC Scopus Sachgebiete
Electronic, Optical and Magnetic Materials, Atomic and Molecular Physics, and Optics, Electrical and Electronic Engineering, Biotechnology
Link zum Portal
https://ucrisportal.univie.ac.at/de/publications/ce3bb7c7-a60c-4af2-bf20-c63f51c376bc