MoS/WSe vdW Heterostructures Decorated with PbS Quantum Dots for the Development of High-Performance Photovoltaic and Broadband Photodiodes.

van der Waals heterostructures (vdWHs) overcoming the lattice and processing limitations of conventional heterostructures provide an opportunity to develop high-performance 2D vdWH solar cells and photodiodes. However, it is challenging to improve the sensitivity and response speed of 2D vdWH photovoltaic devices due to the low light absorption efficiency and electron/hole traps in heterointerfaces. Here, we design a PbS/MoS/WSe heterostructure photodiode in which a light-sensitive PbS quantum dot (QD) layer combined with a MoS/WSe heterostructure significantly enhances the photovoltaic response. The electron current in the heterostructure is increased by the effective collection of photogenerated electrons induced by PbS QDs. The device exhibits a broadband photovoltaic response from 405 to 1064 nm with a maximum responsivity of 0.76 A/W and a specific detectivity of 5.15 × 10 Jones. In particular, the response speed is not limited by multiple electron traps in the PbS QDs/2D material heterointerface, and a fast rising/decaying time of 43/48 μs and a -3 dB cutoff frequency of over 10 kHz are achieved. The negative differential capacitance and frequency dependence of capacitance demonstrate the presence of interface states in the MoS/WSe heterointerface that hamper the improvement of the response speed. The scheme to enhance photovoltaic performance without sacrificing response speed provides opportunities for the development of high-performance 2D vdWH optoelectronic devices.