Growth of centimeter-scale perovskite single-crystalline thin film via surface engineering

Modern electronic and photonic devices rely on single-crystalline thin film semiconductors for high performance and reproducibility. The emerging halide perovskites have extraordinary electronic and photonic properties and can be synthesized via low cost solution-based methods. They have been used in a variety of devices with performance approaching or over the devices based on conventional materials. However, their solution based growth method is intrinsically challenge to grow large scale single-crystalline thin film due to the random nucleation and isotropous growth of the crystal. Here, we report the growth of centimeter-scale perovskite single-crystalline thin films by controlling the nucleation density and growth rate of the crystal under a spatially confined growth condition. The hydrophobic treatment on substrates inhibits nucleation and accelerates the growth of single-crystalline thin film, providing enough space for initial nucleus growing up quickly without touching each other. Single-crystalline perovskite thin-film with an aspect ratio of 1000 (1 cm in side length, 10 μm in thickness) has been successfully grown. The low trap density and the high mobility of the as-grown thin film show a high crystallinity. The photodetector based on the perovskite thin film has achieved a gain ~ 10⁴, benefitting from the short transit time of the carries due to the high mobility and thin thickness of the active layer. Our work opens up a new route to grow large scale perovskite single-crystalline thin films, providing a platform to develop high- performance devices.