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.