Photogalvanic effect in Weyl semimetals from first principles

Using first-principles calculations, we investigate the photogalvanic effect in the Weyl semimetal material TaAs. We find colossal photocurrents caused by the Weyl points in the band structure in a wide range of laser frequency. Our calculations reveal that the photocurrent is predominantly contributed by the three-band transition from the occupied Weyl band to the empty Weyl band via an intermediate band away from the Weyl cone, for excitations both by linearly and circularly polarized light. Therefore, it is essential to sum over all three-band transitions by considering a full set of Bloch bands (both Weyl bands and trivial bands) in the first-principles band structure while it does not suffice to only consider the two-band direct transition within a Weyl cone. The calculated photoconductivities are well consistent with recent experiment measurements. Our work provides a first-principles calculation on nonlinear optical phenomena of Weyl semimetals and provides a deeper understanding of the photogalvanic effects in complexed materials.