Identifying Vibrations that Control Non-adiabatic Relaxation of Polaritons in Strongly Coupled Molecule-Cavity Systems
Tichauer, R. H., Morozov, D., Sokolovskii, I., Toppari, J. J., & Groenhof, G. (2022). Identifying Vibrations that Control Non-adiabatic Relaxation of Polaritons in Strongly Coupled Molecule-Cavity Systems. Journal of Physical Chemistry Letters, 13(26), 6259-6267. https://doi.org/10.1021/acs.jpclett.2c00826
Published inJournal of Physical Chemistry Letters
© 2022 the Authors
The strong light–matter coupling regime, in which excitations of materials hybridize with excitations of confined light modes into polaritons, holds great promise in various areas of science and technology. A key aspect for all applications of polaritonic chemistry is the relaxation into the lower polaritonic states. Polariton relaxation is speculated to involve two separate processes: vibrationally assisted scattering (VAS) and radiative pumping (RP), but the driving forces underlying these two mechanisms are not fully understood. To provide mechanistic insights, we performed multiscale molecular dynamics simulations of tetracene molecules strongly coupled to the confined light modes of an optical cavity. The results suggest that both mechanisms are driven by the same molecular vibrations that induce relaxation through nonadiabatic coupling between dark states and polaritonic states. Identifying these vibrational modes provides a rationale for enhanced relaxation into the lower polariton when the cavity detuning is resonant with specific vibrational transitions. ...
PublisherAmerican Chemical Society (ACS)
Publication in research information system
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Related funder(s)European Commission; Academy of Finland
Funding program(s)Academy Project, AoF
The content of the publication reflects only the author’s view. The funder is not responsible for any use that may be made of the information it contains.
Additional information about fundingThis work was supported by the Academy of Finland (Grant 323996) and European Union (H2020-INFRAEDI-02-2018-823830).
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