The quadratic density response function for non-interacting fermions at arbitrary temperature

Abstract

We develop and implement the quadratic density response function of non-interacting fermions at arbitrary temperature, frequencies, and wave vectors. Starting from a Green's function formulation, we derive the quadratic response and demonstrate its equivalence to the result obtained from the Wigner equation. We further derive the classical limit through a perturbative expansion of the Vlasov equation and demonstrate that the quantum and classical formulations agree in the high-temperature limit. We analyse the limiting behaviour with respect to wavenumber and derive the zeroth harmonic response. Two independent implementations are provided and extensively benchmarked against density-functional theory, canonical path integral Monte Carlo (PIMC), and grand canonical PIMC simulations. As the density response of the interacting electron gas is commonly modelled through the ideal response functions and approximate models for the local field correction, the presented formulation will also allow for more complete explorations of interacting systems. Especially, our efficient implementation, which evaluates the ideal static and dynamic quadratic response functions in less than 0.5 ms on a 1.3 GHz processor, will enable evaluation of quadratic corrections to integrated quantities such as interaction potentials and stopping powers in warm dense matter.