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Qian, Qingkai; Wu, Wenjing; Peng, Lintao; Wang, Yuanxi; Tan, Anne Marie Z.; Liang, Liangbo; Hus, Saban M.; Wang, Ke; Choudhury, Tanushree H.; Redwing, Joan M.; Puretzky, Alexander A.; Geohegan, David B.; Hennig, Richard G.; Ma, Xuedan; Huang, Shengxi
ACS nano, 05/2022, Letnik: 16, Številka: 5Journal Article
The electronic and optical properties of two-dimensional materials can be strongly influenced by defects, some of which can find significant implementations, such as controllable doping, prolonged valley lifetime, and single-photon emissions. In this work, we demonstrate that defects created by remote N2 plasma exposure in single-layer WS2 can induce a distinct low-energy photoluminescence (PL) peak at 1.59 eV, which is in sharp contrast to that caused by remote Ar plasma. This PL peak has a critical requirement on the N2 plasma exposure dose, which is strongest for WS2 with about 2.0% sulfur deficiencies (including substitutions and vacancies) and vanishes at 5.6% or higher sulfur deficiencies. Both experiments and first-principles calculations suggest that this 1.59 eV PL peak is caused by defects related to the sulfur substitutions by nitrogen, even though low-temperature PL measurements also reveal that not all the sulfur vacancies are remedied by the substitutional nitrogen. The distinct low-energy PL peak suggests that the substitutional nitrogen defect in single-layer WS2 can potentially serve as an isolated artificial atom for creating single-photon emitters, and its intensity can also be used to monitor the doping concentrations of substitutional nitrogen.
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