期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 11, 期 7, 页码 2667-2674出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c00247
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资金
- Gordon and Betty Moore Foundation [GBMF7114]
- Princeton Center for Complex Materials
- National Science Foundation (NSF)-MRSEC program [DMR-1420541]
- National Science Foundation [DGE-1656466]
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-SC0012458]
- European Union's H2020 Marie Sklodowska Curie actions [799408]
- European Commission through the European Research Council (ERC), Project INCEPT [677488]
Strong light-matter coupling is emerging as a fascinating way to tune optical properties and modify the photophysics of molecular systems. In this work, we studied a molecular chromophore under strong coupling with the optical mode of a Fabry-Perot cavity resonant to the first electronic absorption band. Using femtosecond pump-probe spectroscopy, we investigated the transient response of the cavity-coupled molecules upon photoexcitation resonant to the upper and lower polaritons. We identified an excited state absorption from upper and lower polaritons to a state at the energy of the second cavity mode. Quantum mechanical calculations of the many-molecule energy structure of cavity polaritons suggest assignment of this state as a two-particle polaritonic state with optically allowed transitions from the upper and lower polaritons. We provide new physical insight into the role of two-particle polaritonic states in explaining transient signatures in hybrid light-matter coupling systems consistent with analogous many-body systems.
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