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The realization of high-performance two-dimensional (2D) solar photovoltaicsystems are both fundamentally intriguing and practically appealing to meet thefast-growing energy requirements. Since the limited application of single 2Dcrystals in photovoltaic, here we propose a family of 2D KAgSe/KAgX(X=S,Te) vander Waals heterostructures (vdWHs), which are constructed by combining twodifferent KAgX layers through interlayer vdW interaction. After a systematicstudy and further regulatory research of these vdWHs based on thefirst-principles, numerous fascinating characteristics and physical mechanismsare obtained. Firstly, favorable potential applications of these vdWHs inphotovoltaics are confirmed in virtue of their desirable optoelectronicproperties, such as the robust stabilitis, moderate direct band gaps, type-IIband alignments together with superior carrier mobilities, visible opticalabsorptions, power conversion efficiencys (PCEs) and photocurrents in theirbased photovoltaic devices. More importantly, when under varying verticalelectric field Ez, a phase transition of band alignment from type-II to type-Iof these vdWHs can be induced by the opposite band shifts between layers, whichmay enrich their applications in light-emitting diodes and lasers. Meanwhile,the PCE can be expanded up to 23%, and an obvious red-shift peak of thephotocurrent in the visible light range are also obtained at different Ez.These fascinating tunable properties of KAgSe/KAgX vdWHs under varying Ez notonly promote the improvement of their photoelectric performances, but theunderlying mechanisms can also be applied to next experimental design andpractical application of other 2D photovoltaic systems. Especially for thered-shift peak of the photocurrent, which is rarely found but highly desirablein practical visible photoelectric conversion.

Design and manipulation of high-performance photovoltaic systems based on two-dimensional novel KAgSe/KAgX(X=S,Te) van der Waals heterojunctions