Large Bulk Photovoltaic Effect and Spontaneous Polarization of Single-Layer Monochalcogenides

We use a first-principles density functional theory approach to calculate the shift current and linear absorption of uniformly illuminated single-layer Ge and Sn monochalcogenides. We predict strong absorption in the visible spectrum and a large effective three-dimensional shift current (∼100μA/V2), larger than has been previously observed in other polar systems. Moreover, we show that the integral of the shift-current tensor is correlated to the large spontaneous effective three-dimensional electric polarization (∼1.9C/m2). Our calculations indicate that the shift current will be largest in the visible spectrum, suggesting that these monochalcogenides may be promising for polar optoelectronic devices. A Rice-Mele tight-binding model is used to rationalize the shift-current response for these systems, and its dependence on polarization, in general terms with implications for other polar materials