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Area of Science:

  • Quantum dynamics
  • Molecular spectroscopy
  • Cavity quantum electrodynamics

Background:

  • Ultrafast nonradiative relaxation is crucial for understanding energy dissipation in molecular systems.
  • Light-matter interactions in optical cavities can modify molecular properties.
  • The behavior of molecular ensembles differs from single molecules.

Purpose of the Study:

  • To theoretically investigate the ultrafast nonradiative relaxation of a molecular ensemble coupled to a cavity mode.
  • To determine how the number of molecules affects relaxation rates.
  • To explore the role of polaritonic states and vibronic coupling.

Main Methods:

  • Real-time quantum dynamics simulations.
  • Theoretical analysis of light-matter interactions.
  • Investigation of (pseudo-)Jahn-Teller interactions in molecular ensembles.

Main Results:

  • Nonradiative relaxation rate strongly depends on the number of coupled molecules (N).
  • Coupling between bright and dark polaritonic states leads to (pseudo-)Jahn-Teller interactions.
  • Collective conical intersection crossings occur for N>2 molecules, facilitating decay.

Conclusions:

  • The number of molecules is a critical factor in controlling ultrafast nonradiative relaxation in cavity systems.
  • Vibronic coupling and collective molecular coordinates govern relaxation pathways.
  • Conical intersections provide efficient routes for energy dissipation from upper polaritons.