Polariton Transitions in Femtosecond Transient Absorption Studies of Ultrastrong Light-Molecule Coupling
Delpo CA, Kudisch B, Park KH, Khan SUZ, Fassioli F, Fausti D, Rand BP, Scholes GD (2020)
Publication Type: Journal article
Publication year: 2020
Journal
Book Volume: 11
Pages Range: 2667-2674
Journal Issue: 7
DOI: 10.1021/acs.jpclett.0c00247
Abstract
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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APA:
Delpo, C.A., Kudisch, B., Park, K.H., Khan, S.-U.-Z., Fassioli, F., Fausti, D.,... Scholes, G.D. (2020). Polariton Transitions in Femtosecond Transient Absorption Studies of Ultrastrong Light-Molecule Coupling. Journal of Physical Chemistry Letters, 11(7), 2667-2674. https://dx.doi.org/10.1021/acs.jpclett.0c00247
MLA:
Delpo, Courtney A., et al. "Polariton Transitions in Femtosecond Transient Absorption Studies of Ultrastrong Light-Molecule Coupling." Journal of Physical Chemistry Letters 11.7 (2020): 2667-2674.
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