Nonmagnetic vacancy engineering for enhanced spin-orbit and valley splitting in van der Waals heterostructures
Phys. Rev. B 113, 115305 – Published 9 March, 2026
DOI: https://doi.org/10.1103/dx2q-x449
Abstract
The development of predictive theories for spin and valley properties in heterostructures requires fundamental understanding of nonmagnetic vacancy effects. Using density functional theory calculations, we find that nonmagnetic vacancies significantly enhance the spin-orbit splitting at the and ′ valleys in the conduction band minimum of monolayer (78.2 meV for W vacancies). However, valley splitting remains prohibited due to preserved time-reversal symmetry. By constructing a van der Waals heterostructure with a monolayer magnetic substrate induces weak exchange interactions, generating a minor valley splitting (−0.8 meV). Remarkably, vacancy engineering amplifies this effect: sulfur vacancies () induce valley splitting ranging from 3.2 to 9.0 meV, while specific tungsten vacancies () achieve a maximum valley splitting of 13.2 meV. Our findings reveal that vacancy-induced orbital hybridization and asymmetric potential gradients enhance Rashba spin-orbit coupling. Furthermore, the combining between nonmagnetic vacancy symmetry in and weak magnetic exchange from establishes an unconventional symmetry protection mechanism for valley splitting enhancement. This defect engineering strategy provides a pathway for designing tunable valleytronic and spintronic devices based on vertical heterojunctions via precise atomic-scale defect control.