Liquid Epitaxial Growth of Two-dimensional Non-layer structured hybrid Perovskite

The hybrid perovskite CH3NH3PbX3 (X= Cl, Br, I) is a promising material for developing novel optoelectronic devices. Owing to the intrinsic non-layer structure, it remains challenging to synthesize molecularly thin CH3NH3PbX3 with large size. Here, we report a low-cost and highly efficient fabrication route to obtain large-scale single-crystalline 2D CH3NH3PbX3 perovskites on a mica substrate via liquid epitaxy. The 2D perovskite is characterized as 8 nm in thickness and hundreds of micrometers in lateral size. First-principles calculations suggest the strong potassium-halogen interactions at the perovskite/mica interface lower the interface energy of perovskites, driving their fast in-plane growth. Spectroscopic investigations reveal 2D CH3NH3PbBr3 possess small exciton binding energy of 30 meV, allowing a superior visible-light photodetector with a photoresponsivity of 126 A/W and a bandwidth exceeded 80 kHz. These features demonstrate that liquid epitaxy is a bottom-up approach to fabricate the non-layer structured 2D perovskites, which offer a new material platform for the device applications and fundamental investigations.