Femtosecond Photophysics of Molecular Polaritons

Abstract

Molecular polaritons are hybrid states of photonic and molecular character that form when molecules strongly interact with light. Strong coupling tunes energy levels and importantly, can modify molecular properties (e.g. photoreaction rates) opening an avenue for novel polariton chemistry. In this perspective, we focus on the collective aspects of strongly coupled molecular systems and how this pertains to the dynamical response of such systems, which though of key importance for attaining modified function under polariton formation, is still not well understood. We discuss how the ultrafast time and spectral resolution make pump-probe spectroscopy an ideal tool to reveal the energy transfer pathways from polariton states to other molecular states of functional interest. Finally, we illustrate how analyzing the free (rather than electronic) energy structure in molecular polariton systems may provide new clues into how energy flows and thus how strong coupling may be exploited.

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Cited by in corpus (6)

• Collective Polaritonic Effects on Chemical Dynamics Suppressed by Disorder
• Ultrafast collapse of molecular polaritons in photoswitch-nanoantennas at room temperature
• Nonlinear semiclassical spectroscopy of ultrafast molecular polariton dynamics
• Evidence for Polariton-Mediated Biexciton Transition in Single-Walled Carbon Nanotubes
• Phonon-Polaritons in Non-Centrosymmetric Systems: Theory of Terahertz Pump-Optical Probe Spectroscopy
• Linear and nonlinear vibrational excitation driven by molecular polaritons