Engineering Cavity Singlet Fission in Rubrene

By employing the numerically exact multiple Davydov D2 ansatz, we study cavity-manipulated singlet fission that is mediated by polaritonic conical intersections for both one- and two-molecule systems. The population evolution of the TT state and the cavity photons is carefully examined in search for...

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Bibliographic Details
Published in:The journal of physical chemistry letters 2022-05, Vol.13 (18), p.4090-4097
Main Authors: Sun, Kewei, Gelin, Maxim F., Zhao, Yang
Format: Article
Language:English
Subjects:
Physical Insights into Light Interacting with Matter
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Summary:By employing the numerically exact multiple Davydov D2 ansatz, we study cavity-manipulated singlet fission that is mediated by polaritonic conical intersections for both one- and two-molecule systems. The population evolution of the TT state and the cavity photons is carefully examined in search for a high fission efficiency via cavity engineering. Several interesting mechanisms have been uncovered, such as photon-assisted singlet fission, system localization via a displaced photon state, and collective enhancement of the fission efficiency for the two-molecule system. It is also found that the system localization process in the two-molecule system differs substantially from that in the one-molecule system because of the appearance of a novel central polaritonic conical intersection in the two-molecule system. It has been demonstrated that the cavity-controlled singlet fission process can be switched on and off by controlling the average pumping photon number.
ISSN:1948-7185
1948-7185
DOI:10.1021/acs.jpclett.2c00801