Interfacial interactions and enhanced optoelectronic properties of GaN/perovskite heterostructures: insight from first-principles calculations

In this study, we explored the structural, electronic, optical, and transport properties of the GaN/perovskite heterostructures using density functional theory combined with non-equilibrium Green’s function calculations. Four interfacial configurations have been studied, and the interfacial properties were discussed on the basis of the optimal theoretical situation. The Ga-polar N-termination interface was found to be the most favorable interfacial configuration, with an interfacial cohesive energy of 0.4 eV/Å 2 , whereas that of the other three heterostructures was less than 0.1 eV/Å 2 . Results showed that the interfacial nitrogen atoms had a significant impact on the structural stability and electronic properties via interfacial hybridizations. Furthermore, the influence of segregated dopants at the interface on device performance was also studied. The interfacial doping strategy proposed in this study demonstrated improved optoelectronic properties. Therefore, these results provide theoretical guidelines for developing high-performance of GaN/perovskite heterostructures in perovskite solar cells. Graphical abstract The atomic structure, electronic and optical properties of GaN (0001)/MAPbI3 (110) interfaces with a lattice mismatch less than 3% were analyzed using first-principles calculations.