Two-Dimensional Halide Perovskites: Tuning Electronic Activities of Defects.
Two-dimensional (2D) halide perovskites are emerging as promising candidates for nanoelectronics and optoelectronics. To realize their full potential, it is important to understand the role of those defects that can strongly impact material properties. In contrast to other popular 2D semiconductors (e.g., transition metal dichalcogenides MX2) for which defects typically induce harmful traps, we show that the electronic activities of defects in 2D perovskites are significantly tunable. For example, even with a fixed lattice orientation one can change the synthesis conditions to convert a line defect (edge or grain boundary) from electron acceptor to inactive site without deep gap states. We show that this difference originates from the enhanced ionic bonding in these perovskites compared with MX2. The donors tend to have high formation energies and the harmful defects are difficult to form at a low halide chemical potential. Thus, we unveil unique properties of defects in 2D perovskites and suggest practical routes to improve them.
Materials and Process Simulation Center and ‡The Resnick Sustainability Institute, California Institute of Technology , Pasadena, California 91125, United States.
Yuanyue
Y
Liu
Materials and Process Simulation Center and ‡The Resnick Sustainability Institute, California Institute of Technology , Pasadena, California 91125, United States.
Hai
H
Xiao
Materials and Process Simulation Center and ‡The Resnick Sustainability Institute, California Institute of Technology , Pasadena, California 91125, United States.
William A
WA
Goddard
Halide perovskites; defects; first-principle calculations; two-dimensional materials