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Area of Science:

  • Physical Chemistry
  • Quantum Optics
  • Materials Science

Background:

  • Strong coupling between molecules and plasmonic nanoparticles forms plexcitons, hybrid light-matter eigenstates.
  • Plexcitons significantly influence molecular electron dynamics, photophysics, and reactivity.
  • Controlling molecular excited states via light-induced interactions is a key research area.

Purpose of the Study:

  • To develop and compare semiclassical and full-quantum theoretical approaches for simulating plexciton dynamics.
  • To investigate the real-time electronic dynamics of plexcitons, including plasmonic dissipative losses.
  • To analyze the differences between quantum and semiclassical models under various interaction regimes.

Main Methods:

  • Combined ab initio molecular description with classical/quantum modeling of plasmonic nanostructures.
  • Employed the stochastic Schrödinger equation for theoretical modeling.
  • Developed and implemented both semiclassical and full-quantum simulation approaches.

Main Results:

  • Presented two distinct theoretical frameworks: one semiclassical and one full-quantum.
  • Successfully simulated the real-time electronic dynamics of plexcitons, incorporating plasmonic losses.
  • Demonstrated numerically and theoretically that even in the weak-field and weak-coupling limit, a small but observable difference emerges between the full-quantum and semiclassical models.

Conclusions:

  • The developed theoretical models provide accurate insights into plexciton dynamics.
  • The study highlights the importance of quantum effects in plexciton behavior, even under weak interaction conditions.
  • These findings advance the understanding of light-matter interactions for potential applications in controlling molecular properties.