Polariton Transitions in Femtosecond Transient Absorption Studies of Ultrastrong Light-Molecule Coupling.
2020
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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