Defect Healing of MAPbI₃ Perovskite Single Crystal Surface by Benzylamine

Abstract

Controlling the surface traps in metal halide perovskites (MHPs) is essential for device performance, stability, and commercialization. Here, a facile approach is introduced to passivate the methylammonium lead iodide (MAPbI3) perovskite single crystal (PSC) surface defects by benzylamine (BA) ligand treatment, and the natural crystallographic (100) facets surface of PSC is chosen as the research platform to provide a deeper understanding of the passivation process. The confocal photoluminescence (PL) results show that the pristine three-dimensional (3D) MAPbI3 PSC surface with a symmetric emission spectrum is normally converted to a pure two-dimensional (2D) BA2PbI4, and also forms a quasi-2D Ruddlesden–Popper perovskite (RPP) BA2MAn−1PbnI3n+1 (n = 2, 3, 4, … ∞) after BA exchange with cation defects. The blue shift in the PL peak, as well as the extended exciton lifetimes of time-resolved photoluminescence (TRPL), indicate the realization of surface defect passivation. Additionally, changes in surface morphology are also investigated. The reaction starts with the formation of small, layered crystallites over the surface; as time elapses, the layered crystallites spread and merge in contact with each other, eventually resulting in smooth features. Our findings present a simple approach for MAPbI3 PSC surface defect passivation, which aims to advance MHP optimization processes toward practical perovskite device applications.

Keywords

• defect passivation
• perovskite single crystal
• photoluminescence
• 2D/3D