The combination of specific van der Waals semiconductors in vertical stacks leads to atomically sharp heterointerfaces with unique properties, offering versatility and additional functionality for thin, flexible, optoelectronic devices. In this work, we demonstrate heterostructures built from single-layer MoS2 (n-type) and multilayer FePS3 (p-type) as multifunctional p-n junctions where robust photoluminescent light emission and broadband electrical photo-response coexist. This is made possible by the inherent properties of the materials involved and the precise energy band alignment at their interface, which preserves the photoluminescent emission provided by the single-layer MoS2 and confers exceptional tunability to the system. Indeed, through small changes in the applied voltage across the junction, the interplay between photoluminescence and photocurrent generation can be tuned, allowing for a precise control of the light emission of single-layer MoS2 - from severely quenched to an order of magnitude enhancement. Additionally, the broadband photo-response of the system presents an enhanced performance under ultraviolet illumination, in contrast to other van der Waals heterostacks containing single-layer semiconductors. Furthermore, this photo-response can be adjusted by the application of an external electric field, enabling photocurrent generation under both reverse and forward bias, thereby contributing to the overall functionality and versatility of the system.
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