Heterogeneity at multiple length scales in halide perovskite semiconductors

Abstract

Materials with highly crystalline lattice structures and low defect concentrations have classically been considered essential for high-performance optoelectronic devices. However, the emergence of high-efficiency devices based on halide perovskites is provoking researchers to rethink this traditional picture, as the heterogeneity in several properties within these materials occurs on a series of length scales. Perovskites are typically fabricated crudely through simple processing techniques, which leads to large local fluctuations in defect density, lattice structure, chemistry and bandgap that appear on short length scales ( 10 μm). Despite these variable and complex non-uniformities, perovskites maintain exceptional device efficiencies and are, as of 2018, the best-performing polycrystalline thin-film solar cell material. In this Review, we highlight the multiple layers of heterogeneity ascertained using high-spatial-resolution methods that provide access to the relevant length scales. We discuss the impact that the optoelectronic variations have on halide perovskite devices, including the prospect that it is this very disorder that leads to their remarkable power-conversion efficiencies. Despite their excellent macroscopic operational parameters, halide perovskites exhibit heterogeneity in materials properties at all lateral and vertical length scales. In this Review, we discuss the nature of heterogeneity in halide perovskites and assess the impact of these non-uniformities on their optoelectronic properties and how the heterogeneity may even be beneficial for device properties.