Properties at the interface of the pristine CdSe and core-shell CdSe-ZnS quantum dots with ultrathin monolayers of two-dimensional MX (M: Mo, W; X: S, Se, Te) heterostructures from density functional theory.

In this work, eight van der Waals heterojunctions based on CdSe or CdSe-ZnS quantum dots (QDs) and four commonly used two-dimensional transition metal dichalcogenides (2D-TMDs) are theoretically designed. On the basis of the constructed structures, density functional theory (DFT) method is employed to investigate the structural and optoelectronic related properties of these heterojunctions in detail. Specifically, their electronic properties including charge density differences, density of states, and band offsets are calculated, based on which band alignment types as well as their potentials as novel photovoltaic materials are discussed. According to these calculations, we proposed that several van der Waals heterostructures including MoS/CdSe, MoTe/CdSe, WSe/CdSe, MoTe/CdSe-ZnS, and WSe/CdSe-ZnS might be used as potential photovoltaic materials due to their type II band alignment characteristics. Moreover, the WSe/CdSe-ZnS heterostructure is expected to have optimal photovoltaic performance attributed to their large bond offsets and band gaps, which could not only facilitate charge separation processes, but also slow down charge recombination. Our present theoretical work could be helpful for the future experimental design of novel CdSe QDs and 2D-TMD based van der Waals heterostructures with excellent photovoltaic performances.