Efficient absolute interface energy calculations for heterostructures: Synergy between localized basis sets, large vacuum, and surface passivation techniques

Heterostructures combining diverse physico-chemical properties are increasingly in demand for a wide range of applications in modern science and technology. However, despite their importance in materials science, accurately determining absolute interface energies remains a major challenge. Here, we present a computationally efficient framework for determining interface energies and their dependencies with chemical potential by incorporating a surface-passivation technique, demonstrated using pseudo-H* passivation combined with an optimized localized-basis-set method. This framework is applied to calculate absolute interface energies and to analyze the electronic properties of both quasi-lattice-matched and lattice-mismatched III–V/Si interfaces, with the results compared to conventional reconstructed-surface calculations. By combining localized basis sets with large vacuum and surface passivation techniques, this approach allows for accurate estimation of absolute interface energies over the whole thermodynamic stability range in heterogeneous material systems. Notably, this framework demonstrates significant potential for providing robust and reliable heterointerface modeling across diverse nanoscale material systems, with direct benchmarking against plane-wave calculations revealing up to 25 times faster computational performance.