First-principles calculation of the bulk photovoltaic effect in the polar compounds LiAsS2, LiAsSe2, and NaAsSe2.

Abstract

We calculate the shift current response, which has been identified as the dominant mechanism for the bulk photovoltaic effect, for the polar compounds LiAsS2, LiAsSe2, and NaAsSe2. We find that the magnitudes of the photovoltaic responses in the visible range for these compounds exceed the maximum response obtained for BiFeO3 by 10-20 times. We correlate the high shift current response with the existence of p states at both the valence and conduction band edges, as well as the dispersion of these bands, while also showing that high polarization is not a requirement. With low experimental band gaps of less than 2 eV and high shift current response, these materials have potential for use as bulk photovoltaics.