Ab Initio Simulation of ZnO/LaMnO₃ Heterojunctions: Insights into Their Structural and Electronic Properties

Layered oxide heterostructures show interesting properties that encompass those of the standalone moieties; hence, a detailed understanding of the interface is key to the development and use of such materials. In this work, we have performed quantum-chemical ab initio calculations to give a complex description of structural and electronic properties of epitaxial growth ZnO/LaMnO₃ (ZnO/LMO) interfaces. The Crystal code, which uses a local (Gaussian) basis set, is used to design and characterize ZnO/LMO heterostructures including (112̅0) and (101̅0) nonpolar overlayers of ZnO on LMO(001), supported from simpler formulation to hybrid functionals of density functional theory. The applied structural models and coincidence cells are described and illustrated in detail. We discuss the impact of different termination of LMO through stability (computed strain and adhesion energies) and structural and electronic properties (density of states and 3D charge density differences). The ZnO(112̅0) overlayer shows the lesser structural distortion and the most stable configuration with LaO termination of LMO. These important findings enable us to propose novel hybrid composites for electrochemical devices