Two-dimensional layered semiconductors have attracted intense interest in recent years. The van der Waals coupling between the layers tolerates stacking various materials and establishing heterostructures with new characteristics for a wide range of optoelectronic applications. The interlayer exciton dynamics at the interface within the heterostructure are vitally important for the performance of the photodetector and photovoltaic device. Here, a heterostructure comprising two-dimensional organic-inorganic Ruddlesden–Popper perovskites and transition metal dichalcogenide monolayer was fabricated and its ultrafast charge separation processes were systematically studied by using femtosecond time-resolved transient absorption spectroscopy. Significant hole and electron transfer processes in the ps and fs magnitude at the interface of the heterostructure were observed by tuning pump wavelengths of the pump-probe geometries. The results emphasize the realization of the exciton devices based on semiconductor heterostructures of two-dimensional perovskite and transition metal dichalcogenide.
