A First-Principles Multiscale Framework for Topological Superconductivity

Abstract: A microscopic understanding of topological superconductivity (TSC) in real materials requires a materials-informed approach that integrates first-principles electronic structure, superconductivity, and topology within a unified computational framework. Here, we develop such an approach by combining density functional theory, Wannier-based low-energy Hamiltonians, Bogoliubov-de Gennes theory, and Matsubara Green's-function-based Chern number calculations performed directly on realistic multiorbital superconducting Hamiltonians. We apply this framework to bulk-like and monolayer FeTeSe and to FeSe/GaAs heterostructures, enabling a unified investigation of both intrinsic and proximity-induced topological superconductivity. We identify key electronic-structure ingredients that promote robust TSC, including Rashba-active states near the Fermi level, strong induced superconducting pairing, and substantial orbital hybridization between spin-orbit-active and superconducting sectors. Guided by these design principles, we predict multiple topological superconducting phases in Fe-based materials and demonstrate that FeSe/GaAs heterostructures are particularly promising, exhibiting topological transitions at experimentally accessible chemical potentials and low Zeeman fields. Complementing the theoretical predictions, we demonstrate the growth and structural characterization of FeSe/GaAs heterostructures, establishing the experimental feasibility of the proposed materials platform. Our results provide a quantitative route for engineering and screening candidate Majorana materials and heterostructures directly from realistic electronic structures and establish a foundation for future materials-by-design approaches to topological superconductivity.