Polarized Fock States for Polariton Photochemistry

TL;DR

This paper introduces polarized Fock states to better describe molecule-cavity systems in quantum electrodynamics, revealing new phenomena and enabling control over photochemical reactions beyond traditional models.

Contribution

It presents a novel use of polarized Fock states to analyze and simulate coupled molecule-cavity systems, providing insights beyond the quantum Rabi model and facilitating photon generation and reactivity control.

Findings

Non-orthogonality of polarized Fock states enables multiple photon generation from a single excitation.

Polarized Fock states offer a more intuitive understanding of molecule-cavity interactions.

The approach improves numerical convergence in simulating polariton photochemistry.

Abstract

We use the polarized Fock states to describe the coupled molecule-cavity hybrid system in quantum electrodynamics. The molecular permanent dipoles polarize the photon field by displacing its vector potential, leading to non-orthogonality between the Fock states of two different polarized photon fields. These polarized Fock states allow an intuitive understanding of several new phenomena that go beyond the prediction of the quantum Rabi model, and at the same time, offer numerical convenience to converge the results. We further exploit this non-orthogonality to generate multiple photons from a single electronic excitation (downconversion) and control the photochemical reactivity.