Heavy Mediator at Quantum Dot/Graphene Heterojunction for Efficient Charge Carrier Transfer: Alternative Approach for High-Performance Optoelectronic Devices.

Two-dimensional (2D) material nanocomposites have emerged as a material system for discovering new physical phenomena and developing novel devices. However, because of the low density of states of most two-dimensional materials such as graphene, the heterostructure of nanocomposites suffers from an enhanced depletion region, which can greatly reduce the efficiency of the charge carrier transfer and deteriorate the device performance. To circumvent this difficulty, here we propose an alternative approach by inserting a second 2D mediator with a heavy effective mass having a large density of states in-between the heterojunction of 2D nanocomposites. The mediator can effectively reduce the depletion region and form a type-II band alignment, which can speed up the dissociation of electron-hole pairs and enhance charge carrier transfer. To illustrate the principle, we demonstrate a novel stretchable photodetector based on the combination of graphene/ReS2/perovskite quantum dots. Two-dimensional ReS2 acts as a mediator in-between highly absorbing perovskite quantum dots and a high-mobility graphene channel and a thiol-based linker between the ReS2 and the perovskite. It is found that the optical sensitivity can be enhanced by 22 times. This enhancement was ascribed to the improvement of the charge transfer efficiency as evidenced by optical spectroscopy measurements. The produced photosensors are capable of reaching the highest reported value of photoresponsivity (>107 A W-1) and detectivity compared to previously studied stretchable devices. Mechanical robustness with tolerable strain up to 100% and excellent stability make our device ideal for future wearable electronics.