Probing Light-Induced Conical Intersections by Monitoring Multidimensional Polaritonic Surfaces

Area of Science:

• Quantum Chemistry
• Molecular Dynamics
• Nanophotonics

Background:

• Molecular interactions with nanocavities lead to polaritonic states.
• Light-induced conical intersections govern molecular dynamics.
• Probing these dynamics typically requires external laser pulses.

Purpose of the Study:

• To demonstrate cavity-enabled tracking of molecular dynamics.
• To show nonadiabatic population transfer between polaritonic surfaces.
• To identify a probe-free method for observing light-induced conical intersections.

Main Methods:

• Theoretical modeling of a polyatomic molecule interacting with a nanocavity.
• Simulation of time-resolved ultrafast radiative emission from the cavity.
• Analysis of nuclear wavepacket dynamics and population transfer.

Main Results:

• Ultrafast radiative emission inherently tracks nuclear wavepacket motion on polaritonic surfaces.
• Nonadiabatic population transfer between surfaces is observed via emission.
• This emission acts as a dynamical fingerprint for light-induced conical intersections.

Conclusions:

• Nanocavity polaritons enable intrinsic observation of molecular dynamics.
• Time-resolved emission provides a probe-free method to study conical intersections.
• This approach offers an experimentally accessible route to understanding light-matter interactions.