Mechanism of Oleic Acid-Mediated Sulfur Vacancy Healing in Monolayer WS ₂

We uncover the mechanism behind the enhancement of photoluminescence yield in monolayer WS₂ through oleic acid treatment, a promising scalable strategy for defect healing. By inducing sulfur vacancies through thermal treatment and monitoring the changes in photoluminescence yield and emission spectra, we demonstrate that in contrast to super acids, oleic acid heals the sulfur vacancy by providing substitutional oxygen, instead of hydrogen. Using density functional theory calculations, we provide insight into the underlying mechanism governing the oleic acid-mediated sulfur vacancy healing process. Our findings suggest that effective defect passivation by oxygen doping can be achieved through chemical treatment, opening a pathway for oxygen doping in transition metal dichalcogenides. However, we also highlight the limitations of chemical treatment, which may only lead to small increases in photoluminescence yield beyond a certain point.