期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 13, 期 27, 页码 6259-6267出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.2c00826
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资金
- Academy of Finland [323996]
- European Union [H2020-INFRAEDI-02-2018- 823830]
- Notes
- Academy of Finland (AKA) [323996, 323996] Funding Source: Academy of Finland (AKA)
This study uses multiscale molecular dynamics simulations to investigate the relaxation process of polaritons in tetracene molecules strongly coupled to confined light modes. The results indicate that the relaxation involves vibrationally assisted scattering (VAS) and radiative pumping (RP), both driven by the same molecular vibrations through nonadiabatic coupling between dark states and polaritonic states.
ABSTRACT: 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.
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