Hartree method for molecular polaritons

TL;DR

This paper develops a Hartree-based theoretical framework to study the evolution of molecular polaritons in organic materials with strong light-matter and vibronic interactions, providing insights into their complex quantum dynamics.

Contribution

It introduces a multiconfiguration Hartree approach to model vibration-assisted polariton wavefunctions considering simultaneous strong electronic, vibrational, and photonic couplings.

Findings

Derived equations of motion for polariton wavefunctions with vibrational interactions.

Provided a mean-field Hartree treatment for vibronic and photonic degrees of freedom.

Enhanced understanding of complex light-matter-vibration coupling in organic polaritons.

Abstract

The formation of the composite photonic-excitonic particle, known as a polariton, is a phenomenon emerging in materials possessing strong coupling to light. The organic-based materials besides the strong light-matter coupling also demonstrate strong interaction of electronic and vibrational degrees of freedom. We study the vibration-assisted polariton wavefunction evolution treating both types of interactions as equally strong. Using the multiconfiguration Hartree approach we derive the equations of motion for the polariton wavefunction, where the vibration degrees of freedom interact with the polariton quantum field through the mean-field Hartree term.