Real-Space, Real-Time Approach to Quantum-Electrodynamical Time-Dependent Density Functional Theory

TL;DR

This paper introduces a real-space, real-time method for solving QED-TDDFT equations, enabling detailed simulations of molecules in cavities with applications to optical spectra and high harmonic generation.

Contribution

It presents a novel real-space, real-time computational approach to QED-TDDFT, improving accuracy and applicability for molecules in optical cavities.

Findings

Accurate modeling of light-matter interactions in cavities.

Dependence of energies and spectra on coupling strength and light frequency.

Successful simulation of high harmonic generation in cavity environments.

Abstract

The Quantum-Electrodynamical Time-Dependent Density Functional Theory (QED-TDDFT) equations are solved by time propagating the wave function on a tensor product of a Fock-space and real-space grid. Applications for molecules in cavities show the accuracy of the approach. Examples include the coupling strength and light frequency dependence of the energies, wave functions, optical absorption spectra, and Rabi splitting magnitudes in cavities, as well as a description of high harmonic generation in cavities.