Shift current response in elemental two-dimensional ferroelectrics

Abstract A bulk material without inversion symmetry can generate a direct current under illumination. This interface-free current generation mechanism, referred to as the bulk photovoltaic effect (BPVE), does not rely on p - n junctions. Here, we explore the shift current generation, a major mechanism responsible for the BPVE, in single-element two-dimensional (2D) ferroelectrics represented by phosphorene-like monolayers of As, Sb, and Bi. The strong covalency, small band gap, and large joint density of states afforded by these elemental 2D materials give rise to large shift currents, outperforming many state-of-the-art materials. We find that the shift current, due to its topological nature, depends sensitively on the details of the Bloch wave functions. It is crucial to consider the electronic exchange-correlation potential beyond the generalized gradient approximation as well as the spin-orbit interaction in density functional theory calculations to obtain reliable frequency-dependent shift current responses.