Nonlinear photovoltaic effects in monolayer semiconductor and layered magnetic material hetero-interface with P- and T-symmetry broken system

Stacking two non-polar materials with different inversion- and rotational-symmetries shows unique nonlinear photovoltaic properties, with potential applications such as in next generation solar-cells. These nonlinear photocurrent properties could be further extended with broken time reversal symmetry present in magnetic materials, however, the combination of time reversal and rotation symmetry breaking has not been fully explored. Herein, we investigate the nonlinear photovoltaic responses in van der Waals heterostructure compromising of monolayer semiconductor and layered magnetic material, MoS₂/CrPS₄; a system with broken P- and T-symmetry. We clearly observe the finite spontaneous photocurrent as shift current at the interface of the MoS₂/CrPS₄ heterostructure. Moreover, we demonstrate that the spontaneous photocurrent drastically changes according to the magnetic phases of CrPS₄. The magnetic phase dependent spontaneous nonlinear photocurrent provides a platform for studying nonlinear photoresponses in systems with broken P- and T-symmetry, and the potential development of magnetic controllable photovoltaic devices.