Mixed-dimensional CsPbBr3@ZnO heterostructures for high-performance p-n diodes and photodetectors

Metal halide perovskite materials are an emerging class of solution-processable semiconductors with considerable potential for use in optoelectronic devices1-3. For example, light-emitting diodes (LEDs) based on these materials could see application in flat-panel displays and solid-state lighting, owing to their potential to be made at low cost via facile solution processing, and could provide tunable colours and narrow emission line widths at high photoluminescence quantum yields4-8. However, the highest reported external quantum efficiencies of green- and red-light-emitting perovskite LEDs are around 14 per cent7,9 and 12 per cent8, respectively-still well behind the performance of organic LEDs10-12 and inorganic quantum dot LEDs13. Here we describe visible-light-emitting perovskite LEDs that surpass the quantum efficiency milestone of 20 per cent. This achievement stems from a new strategy for managing the compositional distribution in the device-an approach that simultaneously provides high luminescence and balanced charge injection. Specifically, we mixed a presynthesized CsPbBr3 perovskite with a MABr additive (where MA is CH3NH3), the differing solubilities of which yield sequential crystallization into a CsPbBr3/MABr quasi-core/shell structure. The MABr shell passivates the nonradiative defects that would otherwise be present in CsPbBr3 crystals, boosting the photoluminescence quantum efficiency, while the MABr capping layer enables balanced charge injection. The resulting 20.3 per cent external quantum efficiency represents a substantial step towards the practical application of perovskite LEDs in lighting and display.

The isolation of a growing number of two-dimensional (2D) materials has inspired worldwide efforts to integrate distinct 2D materials into van der Waals (vdW) heterostructures. Given that any passivated, dangling-bond-free surface will interact with another through vdW forces, the vdW heterostructure concept can be extended to include the integration of 2D materials with non-2D materials that adhere primarily through non-covalent interactions. We present a succinct and critical survey of emerging mixed-dimensional (2D + nD, where n is 0, 1 or 3) heterostructure devices. By comparing and contrasting with all-2D vdW heterostructures as well as with competing conventional technologies, we highlight the challenges and opportunities for mixed-dimensional vdW heterostructures.

The p-n junction is the functional element of many electronic and optoelectronic devices, including diodes, bipolar transistors, photodetectors, light-emitting diodes and solar cells. In conventional p-n junctions, the adjacent p- and n-type regions of a semiconductor are formed by chemical doping. Ambipolar semiconductors, such as carbon nanotubes, nanowires and organic molecules, allow for p-n junctions to be configured and modified by electrostatic gating. This electrical control enables a single device to have multiple functionalities. Here, we report ambipolar monolayer WSe2 devices in which two local gates are used to define a p-n junction within the WSe2 sheet. With these electrically tunable p-n junctions, we demonstrate both p-n and n-p diodes with ideality factors better than 2. Under optical excitation, the diodes demonstrate a photodetection responsivity of 210 mA W(-1) and photovoltaic power generation with a peak external quantum efficiency of 0.2%, promising values for a nearly transparent monolayer material in a lateral device geometry. Finally, we demonstrate a light-emitting diode based on monolayer WSe2. These devices provide a building block for ultrathin, flexible and nearly transparent optoelectronic and electronic applications based on ambipolar dichalcogenide materials.