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Valley pseudospin in two-dimensional (2D) transition-metal dichalcogenides(TMDs) allows optical control of spin-valley polarization and intervalleyquantum coherence. Defect states in TMDs give rise to new exciton features andtheoretically exhibit spin-valley polarization; however, experimentalachievement of this phenomenon remains challenges. Here, we report unambiguousvalley pseudospin of defect-bound localized excitons in CVD-grown monolayerMoS2; enhanced valley Zeeman splitting with an effective g-factor of -6.2 isobserved. Our results reveal that all five d-orbitals and the increasedeffective electron mass contribute to the band shift of defect states,demonstrating a new physics of the magnetic responses of defect-bound localizedexcitons, strikingly different from that of A excitons. Our work paves the wayfor the manipulation of the spin-valley degrees of freedom through defectstoward valleytronic devices.

Spin-Valley Locking Effect in Defect States of Monolayer MoS$_2$