Strong coupling between an optical mode and an ensemble of molecular vibrations creates new vibration-cavity polariton modes, whose very presence can strongly modify reaction dynamics even without excitation. The ultrafast nonlinear spectroscopy of the polaritonic system, comprising the polariton modes and a reservoir of dark states, might serve to elucidate the mechanism of the reaction modification as well as shed light on novel applications in photonics. Thus far, studies of ultrafast dynamics under strong coupling have largely been limited to hexacarbonyls in solution. Here, we present our recent results from nitroprusside and thiocyanate ions, which have strong infrared transitions but are distinct from hexacarbonyls in several important respects. We discuss the similarities and differences between the vibration-cavity polariton dynamics in these systems and how the results solidify our understanding of polariton dynamics in general.

Absorber-specific dynamics in vibration-cavity polaritons

ACS Spring 2022

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