Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 17, Pages 7758-7767Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c00921
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Funding
- National Science Foundation [CHE-1953045]
- Chemical Sciences, Geosciences, and Biosciences division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy [DEFG02-04ER15571, DE-SC0022134]
- National Research Foundation of Korea (NRF) grant - Korea government (MSIT) [2021R1C1C2007977]
- National Supercomputing Center [KSC-2021-CRE-0187]
- National Research Foundation of Korea [2021R1C1C2007977] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Optical cavities provide a versatile platform for manipulating the excited-state dynamics of molecules. The study observes a novel polaritonic conical intersection (PCI) and finds that it can significantly change the nonadiabatic dynamics of molecules. Additionally, the absorption spectrum and excited-state dynamics can be systematically manipulated by adjusting the parameters of the optical cavity.
Optical cavities provide a versatile platform for manipulating the excited-state dynamics of molecules via stronglight-matter coupling. We employ optical absorption and two-multidimensional electronic spectroscopy simulations to investigatethe effect of optical cavity coupling in the nonadiabatic dynamics ofphotoexcited pyrazine. We observe the emergence of a novelpolaritonic conical intersection (PCI) between the electronic darkstate and photonic surfaces as the cavity frequency is tuned. The PCIcould significantly change the nonadiabatic dynamics of pyrazine bydoubling the decay rate constant of the S2state population. Moreover, the absorption spectrum and excited-state dynamics could besystematically manipulated by tuning the strong light-matter interaction, e.g., the cavity frequency and cavity coupling strength. We propose that a tunable optical cavity-molecule system may provide promising approaches for manipulating the photophysical properties of molecules
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