Dynamic Response Functions for Cavity Quantum Electrodynamics Hartree–Fock Theory

Abstract Frequency-dependent linear and quadratic response functions are implemented for a cavity quantum electrodynamics (QED) generalization of Hartree–Fock (HF) theory. Dynamic electric dipole polarizability, optical rectification hyperpolarizability, and second harmonic generation hyperpolarizability tensors are evaluated for molecules strongly coupled to a single-mode optical cavity, and the results are benchmarked against the same tensors obtained from real-time time-dependent QED-HF simulations. Substantial cavity-induced changes to the frequency-dependent properties are observed for certain perturbing frequencies at large electron–photon coupling strengths. We also find special perturbing frequencies at which there is no cavity effect, regardless of the coupling strength.