Symmetry Breaking and Spin–Orbit Coupling for Individual Vacancy-Induced In-Gap States in MoS₂ Monolayers

Abstract

Spins confined to point defects in atomically thin semiconductors constitute well-defined atomic-scale quantum systems that are being explored as single-photon emitters and spin qubits. Here, we investigate the in-gap electronic structure of individual sulfur vacancies in molybdenum disulfide (MoS 2 ) monolayers using resonant tunneling scanning probe spectroscopy in the Coulomb blockade regime. Spectroscopic mapping of defect wave functions reveals an interplay of local symmetry breaking by a charge-state-dependent Jahn−Teller lattice distortion that, when combined with strong (≃100 meV) spin−orbit coupling, leads to a locking of an unpaired spin-1/2 magnetic moment to the lattice at low temperature, susceptible to lattice strain. Our results provide new insights into the spin and electronic structure of vacancyinduced in-gap states toward their application as electrically and optically addressable quantum systems.