Aligning Transition Dipole Moment toward Light Amplification and Polarized Emission in Hybrid Perovskites

Abstract Orientational manipulation of transition dipole moment (TDM) plays an important role in controlling the polarization of excited states in light emission as well as lasing actions. The present work discovers vertically aligned TDMs in hybrid perovskite films through angle‐resolved photoluminescence (PL) measurements, which show enhanced emission through the film edge. With increasing excitation intensity, the edge emission induced by these vertically aligned TDMs becomes dominant and eventually leads to amplified spontaneous emission (ASE) through the edge view. Meanwhile, polarized emission of both PL and electroluminescence (EL) provides further evidence for vertically aligned TDMs. Surprisingly, the degree of polarization (DOP) through the film edge is increased when grain boundary defects are passivated through either stochiometric engineering or self‐passivation by mobile ions under working conditions. With increasing DOP, ASE threshold of the perovskite film is reduced owing to enhanced collective behaviors of light‐emitting states. This work presents a useful method to manipulate TDMs in organic–inorganic hybrid perovskites.