Probing Light-Induced Conical Intersections by Monitoring Multidimensional Polaritonic Surfaces

The interaction of a molecule with the quantized electromagnetic field of a nanocavity gives rise to light-induced conical intersections between polaritonic potential energy surfaces. We demonstrate for a realistic model of a polyatomic molecule that the time-resolved ultrafast radiative emission of the cavity enables following both nuclear wavepacket dynamics on, and nonadiabatic population transfer between, polaritonic surfaces without applying a probe pulse. The latter provides an unambiguous (and in principle experimentally accessible) dynamical fingerprint of light-induced conical intersections.

Automated summary

The interaction between a molecule and the quantized electromagnetic field of a nanocavity can create light-induced conical intersections between polaritonic potential energy surfaces. By using time-resolved ultrafast radiative emission of the cavity, we can observe the nuclear wavepacket dynamics and nonadiabatic population transfer between polaritonic surfaces without a probe pulse, providing a clear dynamical fingerprint of light-induced conical intersections.