Design principles for shift current photovoltaics

While the basic principles and limitations of conventional solar cells are well understood, relatively little attention has gone toward maximizing the potential efficiency of photovoltaic devices based on shift currents. In this work, we outline simple design principles for the optimization of shift currents for frequencies near the band gap, derived from the analysis of a general effective model. The use of a novel sum rule allows us to express the band edge shift current in terms of a few model parameters and to show it depends explicitly on wavefunctions via Berry connections in addition to standard band structure. We use our approach to identify two new classes of shift current photovoltaics, ferroelectric polymer films and single-layer orthorhombic monochalcogenides such as GeS. We introduce tight-binding models for these systems, and show that they exhibit the largest shift current responsivities at the band edge reported so far. Moreover, exploring the parameter space of these models we find photoresponsivities that can exceed $100$ mA/W. Our results show how the study of the shift current via effective models allows one to improve the possible efficiency of devices based on this mechanism and better grasp their potential to compete with conventional solar cells.