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A low-temperature electron spin resonance study has been carried out on large-area high-purity polycrystalline two-dimensional few monolayer (ML) 2H MoS 2  films synthesized by sulfurization of Mo layers, with intent to atomically assess mobility-degrading detrimental point defects. This reveals the presence of a distinct previously unreported anisotropic defect of axial symmetry about the  c -axis characterized by  g   //  = 2.00145 and  g   ⊥  = 2.0027, with corresponding density (spin S = ½) ~3 × 10 12  cm −2  for a 4 ML thick film. Inverse correlation of the defect density with grain size points to a domain boundary associated defect, inherently incorporated during sample growth. Based on the analysis of ESR signal features in combination with literature data, the signal is tentatively ascribed to the a (di)sulfur antisite defect (S or S 2  substituting for a Mo atom). Beset by these defects, the grain boundaries thus emerge as an intolerable threat for the carrier mobility and layer functionality.

Paramagnetic Intrinsic Defects in Polycrystalline Large-Area 2D MoS2 Films Grown on SiO2 by Mo Sulfurization