Optoelectronic Properties of a van der Waals WS₂ Monolayer/2D Perovskite Vertical Heterostructure

Two-dimensional (2D) Ruddlesden-Popper perovskites have been demonstrated to possess great potential for optical and optoelectronic devices. Because they exhibit better ambient stability than three-dimensional (3D) perovskites, they have been considered as potential substitutes for 3D perovskites as light absorbing layers to improve the photoresponsivity of monolayer transition metal dichalcogenide (TMDC)-based photodetectors. Investigation of the optoelectronic properties of TMDC monolayer/2D perovskite vertical heterostructures is however at an early stage. Here, we address the photovoltaic effect and the photodetection performance in tungsten disulfide (WS₂) monolayer/2D perovskite (C₆H₅C₂H₄NH₃)₂PbI₄ (PEPI) vertical heterostructures. A vertical device geometry with separate graphene contacts to both heterointerface constituents acted as a photovoltaic device and self-driven photodetector. The photovoltaic device exhibited an open circuit voltage of -0.57 V and a short circuit current of 41.6 nA. A photoresponsivity of 0.13 mA/W at the WS₂/PEPI heterointerface was achieved, which was signified by a factor of 5 compared to that from the individual WS₂ region. The current on/off ratio of the self-driven photodetector was approximately 1500. The photoresponsivity and external quantum efficiency of the self-driven photodetector were estimated to be 24.2 μA/W and 5.7 × 10^-5, respectively. This work corroborates that 2D perovskites are promising light absorbing layers in optoelectronic devices with a TMDC-based heterointerface.