Atomic scale model and electronic structure of Cu$_2$O/CH$_3$NH$_3$PbI$_3$ interfaces in perovskite solar cells

Abstract: Cuprous oxide has been conceived as a potential alternative to traditional organic hole transport layers in hybrid halide perovskite-based solar cells. Device simulations predict record efficiencies using this semiconductor, but experimental results do not yet show this trend. More detailed knowledge about the Cu$_2$O/perovskite interface is mandatory to improve the photoconversion efficiency. Using density functional theory calculations, here we study the interfaces of CH$_3$NH$_3$PbI$_3$ with Cu$_2$O to assess their influence on device performance. Several atomistic models of these interfaces are provided for the first time, considering different compositions of the interface atomic planes. The interface electronic properties are discussed on the basis of the optimal theoretical situation, but in connection with the experimental realizations and device simulations. It is shown that the formation of vacancies in the Cu$_2$O terminating planes is essential to eliminate dangling bonds and trap states. The four interface models that fulfill this condition present a band alignment favorable for photovoltaic conversion. Energy of adhesion, and charge transfer across the interfaces are also studied. The termination of CH$_3$NH$_3$PbI$_3$ in PbI$_2$ atomic planes seems optimal to maximize the photoconversion efficiency.