In Situ Growth Mechanism for High-Quality Hybrid Perovskite Single-Crystal Thin Films with High Area to Thickness Ratio: Looking for the Sweet Spot

The development of in situ growth methods for the fabrication of high-quality perovskite single-crystal thin films (SCTFs) directly on hole-transport layers (HTLs) to boost the performance of optoelectronic devices is critically important. However, the fabrication of large-area high-quality SCTFs with thin thickness still remains a significant challenge due to the elusive growth mechanism of this process. In this work, the influence of three key factors on in situ growth of high-quality large-size MAPbBr₃ SCTFs on HTLs is investigated. An optimal “sweet spot” is determined: low interface energy between the precursor solution and substrate, a slow heating rate, and a moderate precursor solution concentration. As a result, the as-obtained perovskite SCTFs with a thickness of 540 nm achieve a record area to thickness ratio of 1.94 × 10⁴ mm, a record X-ray diffraction peak full width at half maximum of 0.017°, and an ultralong carrier lifetime of 1552 ns. These characteristics enable the as-obtained perovskite SCTFs to exhibit a record carrier mobility of 141 cm² V⁻¹ s⁻¹ and good long-term structural stability over 360 days.