Methylamine-assisted growth of uniaxial-oriented perovskite thin films with millimeter-sized grains

Defects from grain interiors and boundaries of perovskite films cause significant nonradiative recombination energy loss, and thus perovskite films with controlled crystallinity and large grains is critical for improvement of both photovoltaic performance and stability for perovskite-based solar cells. Here, a methylamine (MA⁰) gas-assisted crystallization method is developed for fabrication of methylammonium lead iodide (MAPbI₃) perovskite films. In the process, the perovskite film is formed via controlled release of MA0 gas molecules from a liquid intermediate phase MAPbI₃·xMA⁰. The resulting perovskite film comprises millimeter-sized grains with (110)-uniaxial crystallographic orientation, exhibiting much low trap density, long carrier lifetime, and excellent environmental stability. The corresponding perovskite solar cell exhibits a power conversion efficiency (PCE) of ~ 21.36%, which is among the highest reported for MAPbI₃-based devices. This method provides important progress towards the fabrication of high-quality perovskite thin films for low-cost, highly efficient and stable perovskite solar cells.