Identifying Vibrations that Control Non-adiabatic Relaxation of Polaritons in Strongly Coupled Molecule-Cavity Systems

被引:23
|
作者
Tichauer, Ruth H. [1 ,2 ]
Morozov, Dmitry [1 ,2 ]
Sokolovskii, Ilia [1 ,2 ]
Toppari, J. Jussi [1 ,2 ]
Groenhof, Gerrit [1 ,2 ]
机构
[1] Univ Jyvaskyla, Nanosci Ctr, Jyvaskyla 40014, Finland
[2] Univ Jyvaskyla, Dept Chem, Jyvaskyla 40014, Finland
来源
JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2022年 / 13卷 / 27期
基金
芬兰科学院; 欧盟地平线“2020”;
关键词
SEMICLASSICAL SCATTERING THEORY; DENSITY-FUNCTIONAL THEORY; DYNAMICS; CHEMISTRY; EMISSION; QUANTUM;
D O I
10.1021/acs.jpclett.2c00826
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:6259 / 6267
页数:9
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