Self-regulation mechanism for charged point defects in hybrid halide perovskites

TL;DR

This paper explains how hybrid halide perovskites self-regulate charge carriers through ionic defect formation, which impacts their photovoltaic efficiency, based on quantum mechanical calculations of defect chemistry.

Contribution

It reveals a novel ionic compensation mechanism in perovskites that controls free carrier concentrations, contrasting with traditional inorganic semiconductor defect models.

Findings

Charged vacancy concentration exceeds 0.4% at room temperature

Ionic disorder dominates over electronic disorder in defect regulation

Self-regulation influences photovoltaic performance

Abstract

Hybrid halide perovskites such as methylammonium lead iodide (CH3NH3PbI3) exhibit unusually low free carrier concentrations despite being processed at low-temperatures from solution. We demonstrate, through quantum mechanical calculations, that the origin of this phenomenon is a prevalence of ionic over electronic disorder in stoichiometric materials. Schottky defect formation provides a mechanism to self-regulate the concentration of charge carriers through ionic compensation of charged point defects. The equilibrium charged vacancy concentration is predicted to exceed 0.4% at room temperature. This behaviour, which goes against established defect conventions for inorganic semiconductors, has implications for photovoltaic performance.