Microscopic analysis of high harmonic generation in semiconductors with degenerate bands

TL;DR

This paper introduces a microscopic approach using multiband semiconductor Bloch equations to accurately model high-harmonic generation in semiconductors with degenerate bands, addressing phase ambiguities and band crossing issues.

Contribution

It develops a length gauge method with smooth gauge transformation to handle degenerate bands, validated against velocity gauge calculations, improving computational efficiency and physical interpretability.

Findings

High-harmonic spectra match experimental data for GaAs.

Berry curvature influences even-order harmonics polarization.

Length gauge requires fewer bands and less computation.

Abstract

Based on the multiband semiconductor Bloch equations a microscopic approach to high-harmonic generation in crystalline solids which is able to properly describe degenerate bands and band crossings is presented and analyzed. It is well-known that numerical band structure calculations typically provide electronic wave functions with an undetermined k-dependent phase which results in matrix elements which contain arbitrary k-dependent phases. In addition, such approaches usually mix degenerate bands and bands with an energy difference smaller than the numerical precision in an arbitrary way for each point in k-space. These ambiguities are problematic if one considers the dynamics induced by electric fields since the matrix elements of the position operator involve a derivative of the wave functions with respect to k. When the light-matter interaction is described in the length gauge, the problem of arbitrary phases and degenerate subspace mixing of Bloch states is solved by adopting a smooth gauge transformation along the field direction. The results obtained within this method are validated by comparing with calculations in the velocity gauge. Although we obtain in both gauges the same overall result, the length gauge is advantageous since it converges with a smaller number of bands and thus requires significantly less numerical effort than the velocity gauge. Also an unique distinction between inter- and intraband contributions and thus an instructive physical interpretation is possible in the length gauge whereas in the velocity gauge this is unclear. The computed polarization-direction-dependent high-harmonic spectra agree well with experimental data reported for GaAs. Furthermore, it is demonstrated that, under proper conditions, the Berry curvature is largely responsible for the even-order harmonics which are polarized perpendicular to the driving field.