Protective Coating Interfaces for perovskite Solar Cell Materials: A first Principles Study

TL;DR

This study uses first principles calculations to evaluate inorganic coatings like ZnO, SrZrO3, and ZrO2 for protecting CsPbI3 perovskite surfaces, assessing their atomic structures and electronic level alignments to improve stability and functionality.

Contribution

It provides a detailed first-principles analysis of interface structures and electronic properties of inorganic coatings on CsPbI3, identifying ZrO2 as a potential electron transport layer.

Findings

ZrO2 may serve as an effective electron transport layer.

ZnO and SrZrO3 act as insulators on CsPbI3.

No detrimental mid-gap states are found at the interfaces.

Abstract

The protection of halide perovskites is important for the performance and stability of emergent perovskite-based optoelectronic technologies. In this work, we investigate the potential inorganic protective coating materials ZnO, SrZrO3, and ZrO2 for the CsPbI3perovskite. The optimal interface registries are identified with Bayesian optimization. We then use semi-local density-functional theory (DFT) to determine the atomic structure at the interfaces of each coating material with the clean CsI-terminated surface and three reconstructed surface models with added PbI2and CsI complexes. For the final structures, we explore the level alignment at the interface with hybrid DFT calculations. Our analysis of the level alignment at the coating-substrate interfaces reveals no detrimental mid-gap states, but substrate-dependent valence and conduction band offsets. While ZnO and SrZrO3act as insulators on CsPbI3, ZrO2 might be suitable as electron transport layer with the right interface engineering.