Polymer-Assisted Controllable Growth of Large-Scale and High-Quality Two-Dimensional Perovskite Single-Crystal Microplate Arrays toward Photodetector Integration.

Two-dimensional (2D) hybrid perovskites have come into the spotlight for optoelectronic applications due to their numerous exceptional properties. However, the lack of efficient methods for controllable growth of large-scale and high-quality 2D perovskite single-crystal (PSC) arrays restricts their practical application in integrated optoelectronic devices, such as photoconductor-type photodetector integration. Herein, a polyvinylpyrrolidone (PVP)-assisted template-space-confined method is proposed for growing patterned 2D PSC microplate arrays, in virtue of which a series of 2D PSC microplates in various Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) phases, as well as tunable lateral size and thickness, can be achieved. It is revealed that coordination-bonding interactions between the carbonyl groups of PVP molecules and perovskite precursor ions contribute to the uniform and continuous growth of 2D PSC microplate arrays spanning 100 mm2 areas. Specifically, the (PEA)2PbI4 PSC microplate arrays synthesized with the optimal 4 wt % PVP concentration exhibit high-quality crystallinity and low defect/trap density. In consequence, the photodetector array based on as-grown (PEA)2PbI4 microplate arrays is demonstrated with excellent photodetection performance and low device-to-device variation. This method enables controlling and scaling up the growth of high-quality 2D PSC microplate arrays, which constitutes an important step toward large-scale and integrated optoelectronic systems.