Light-Matter Response in Non-Relativistic Quantum Electrodynamics: Quantum Modifications of Maxwell's Equations

TL;DR

This paper develops a comprehensive linear-response theory for non-relativistic quantum electrodynamics, revealing quantum modifications to Maxwell's equations in matter and enabling ab-initio calculations of light-matter interactions.

Contribution

It introduces a novel framework combining quantum-electrodynamical density-functional theory with a modified RPA to analyze coupled matter-photon responses non-perturbatively.

Findings

Quantum modifications alter Maxwell's equations in matter.

First ab-initio spectra for molecules coupled to quantized fields.

Efficient numerical solution of coupled light-matter response equations.

Abstract

We derive the full linear-response theory for non-relativistic quantum electrodynamics in the long wavelength limit, show quantum modifications of the well-known Maxwell's equation in matter and provide a practical framework to solve the resulting equations by using quantum-electrodynamical density-functional theory. We highlight how the coupling between quantized light and matter changes the usual response functions and introduces new types of cross-correlated light-matter response functions. These cross-correlation responses lead to measurable changes in Maxwell's equations due to the quantum-matter-mediated photon-photon interactions. Key features of treating the combined matter-photon response are that natural lifetimes of excitations become directly accessible from first principles, changes in the electronic structure due to strong light-matter coupling are treated fully non-perturbatively, and for the first time self-consistent solutions of the back-reaction of matter onto the photon vacuum and vice versa are accounted for. By introducing a straightforward extension of the random-phase approximation for the coupled matter-photon problem, we calculate the first ab-initio spectra for a real molecular system that is coupled to the quantized electromagnetic field. Our approach can be solved numerically very efficiently. The presented framework leads to a shift in paradigm by highlighting how electronically excited states arise as a modification of the photon field and that experimentally observed effects are always due to a complex interplay between light and matter. At the same time the findings provide a new route to analyze as well as propose experiments at the interface between quantum chemistry, nanoplasmonics and quantum optics.