Spin-defect characteristics of single sulfur vacancies in monolayer ${\text{MoS}}_2$

Abstract

Single spin defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2 and Q*) of He-ion induced sulfur vacancies in monolayer ${\text{MoS}}_2$. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wavefunction extent of $\sim$ 3.5 nm. The distinct valley-Zeeman splitting in out-of-plane $B$-fields and the brightening of dark states through in-plane $B$-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab-initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

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• Photoemission orbital tomography for excitons in organic molecules
• Self-aligned hybrid nanocavities using atomically thin materials
• First-principles computational methods for quantum defects in two-dimensional materials: A perspective
• All-optical magnetic imaging with spin defects in van der Waals materials at Angstrom-scale
• Orbitally resolved single-photon emission from an individual atomic vacancy center in a semiconductor
• Geometric Percolation Threshold Defines Half-Metallic Window in Vacancy-Doped Titanium disulfides