Microscopic analysis of high harmonic generation in semiconductors with degenerate bands

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 a 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.

Automated summary

A microscopic approach to high-harmonic generation in crystalline solids is presented, which properly describes degenerate bands and band crossings. The length gauge is found to be advantageous over the velocity gauge, requiring less numerical effort and providing a clear distinction between inter- and intraband contributions. The computed high-harmonic spectra agree well with experimental data and demonstrate the importance of the Berry curvature for even-order harmonics.