Including many-body effects into the Wannier-interpolated quadratic photoresponse tensor

TL;DR

This paper introduces a first-principles method to include many-body effects in the quadratic optical response of noncentrosymmetric crystals, enabling accurate predictions of nonlinear optical properties with computational efficiency.

Contribution

It develops a general numerical scheme combining time-dependent current-density response theory with Wannier interpolation to incorporate excitonic effects in quadratic optical responses.

Findings

Excitonic effects cause sharp resonances in second-harmonic generation spectra.

The method achieves good agreement with experimental measurements.

It effectively captures spectral features and angular dependence in various materials.

Abstract

We present a first-principles scheme for incorporating many-body interactions into the unified description of the quadratic optical response to light of noncentrosymmetric crystals. The proposed method is based on time-dependent current-density response theory and includes the electron-hole attraction \textit{via} a tensorial long-range exchange-correlation kernel, which we calculate self-consistently using the bootstrap method. By bridging with the Wannier-interpolation of the independent-particle transition matrix elements, the resulting numerical scheme is very general and allows resolving narrow many-body spectral features at low computational cost. We showcase its potential by inspecting the second-harmonic generation in the benchmark zinc-blende semiconductor GaAs, the layered graphitic semiconductor BC$_{2}$N and the Weyl semimetal TaAs. Our results show that excitonic effects can give rise to large and sharply localized one- and two-photon resonances that are absent in the independent-particle approximation. We find overall good agreement with available experimental measurements, capturing the magnitude and peak-structure of the spectrum as well as the angular dependence at fixed photon energy. The implementation of the method in Wannier-based code packages can serve as a basis for performing accurate theoretical predictions of quadratic optical properties in a vast pool of materials.