Nonlinear Optical and Photocurrent Responses in Janus MoSSe Monolayer and MoS2–MoSSe van der Waals Heterostructure

Two-dimensional (2D) transition metal dichalcogenides are promising materials platforms for a variety of optoelectronic device applications. Janus 2D materials are a rising class of 2D materials with low symmetry, which leads to the emergence of out-of-plane electric polarization and piezoelectricity. Using first-principles density functional theory, we show that monolayer and bilayer heterostructure Janus MoSSe moieties exhibit strong nonlinear optical responses that are vanishing in the non-Janus form. The absence of horizontal mirror plane symmetry enables a circular photocurrent as well as a large out-of-plane second harmonic generation (SHG) and shift photocurrent. Through a comparative study of the Janus heterostructure MoS₂-MoSSe on five distinct stacking configurations, we find that the magnitude of the out-of-plane SHG in the Janus heterostructure is enhanced due to the interlayer coupling and interference effect compared to that of monolayer MoSSe. Thus, Janus 2D materials offer a unique opportunity for exploring nonlinear optical phenomena and designing configurable layered nonlinear optical materials.