Enhanced Photocurrent Owing to Shuttling of Charge Carriers across 4-Aminothiophenol-Functionalized MoSe₂–CsPbBr₃ Nanohybrids

Mixed-dimensional van der Waals nanohybrids (MvNHs) of two-dimensional transition-metal dichalcogenides (TMDs) and zero-dimensional perovskites are highly promising candidates for high-performance photonic device applications. However, the growth of perovskites over the surface of TMDs has been a challenging task due to the distinguishable surface chemistry of these two different classes of materials. Here, we demonstrate a synthetic route for the design of MoSe2–CsPbBr3 MvNHs using a bifunctional ligand, i.e., 4-aminothiophenol. Close contact between these two materials is established via a bridge that leads to the formation of a donor–bridge–acceptor system. The presence of the small conjugated ligand facilitates faster charge diffusion across MoSe2–CsPbBr3 interfaces. Density functional theory calculations confirm the type-II band alignment of the constituents within the MvNHs. The MoSe2–CsPbBr3 nanohybrids show much higher photocurrent (∼2 × 104-fold photo-to-dark current ratio) as compared to both pure CsPbBr3 nanocrystals and pristine MoSe2 nanosheets owing to the synergistic effect of pronounced light–matter interactions followed by efficient charge separation and transportation. This study suggests the use of a bifunctional ligand to construct a nanohybrid system to tune the optoelectronic properties for potential applications in photovoltaic devices.