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

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.

arXiv comment27 pages, 16 figures

References in corpus (7)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Efficient Bayesian Inference of Atomistic Structure in Complex Functional Materials
• Detecting stable adsorbates of (1S)-camphor on Cu(111) with Bayesian optimization
• Integrating Bayesian Inference with Scanning Probe Experiments for Robust Identification of Surface Adsorbate Configurations
• Atomic and electronic structure of cesium lead triiodide surfaces
• Surface reconstruction of tetragonal methylammonium lead triiodide