Sulfur Vacancies In MoS2 Research Articles

Hydrogenated MoS2 QD-TiO2 heterojunction mediated efficient solar hydrogen production.

Herein, we report the development of a hydrogenated MoS2 QD-TiO2 (HMT) heterojunction as an efficient photocatalytic system via a one-pot hydrothermal reaction followed by hydrogenation. This synthetic strategy facilitates the formation of MoS2 QDs with an enhanced band gap and a proper heterojunction between them and TiO2, which accelerates charge transfer process. Hydrogenation leads to oxygen vacancies in TiO2, enhancing the visible light absorption capacity through narrowing its band gap, and sulfur vacancies in MoS2, which enhance the active sites for hydrogen adsorption. Due to the band gap reduction of hydrogenated TiO2 and the band gap enhancement of the MoS2 QDs, the energy states are rearranged to create a reverse movement of electrons and holes facilitated the charge transfer process which enhance life-time of photo-generated charges. The photocatalyst showed stable, efficient and exceptionally high noble metal free sunlight-induced hydrogen production with a maximum rate of 3.1 mmol g-1 h-1. The developed synthetic strategy also provides flexibility towards the shape of the MoS2, e.g. QDs/single or few layers, on TiO2 and offers the opportunity to design novel visible light active photocatalysts for different applications.

Achieving Ultrafast Hole Transfer at the Monolayer MoS2 and CH3NH3PbI3 Perovskite Interface by Defect Engineering.

The performance of a photovoltaic device is strongly dependent on the light harvesting properties of the absorber layer as well as the charge separation at the donor/acceptor interfaces. Atomically thin two-dimensional transition metal dichalcogenides (2-D TMDCs) exhibit strong light-matter interaction, large optical conductivity, and high electron mobility; thus they can be highly promising materials for next-generation ultrathin solar cells and optoelectronics. However, the short optical absorption path inherent in such atomically thin layers limits practical applications. A heterostructure geometry comprising 2-D TMDCs (e.g., MoS2) and a strongly absorbing material with long electron-hole diffusion lengths such as methylammonium lead halide perovskites (CH3NH3PbI3) may overcome this constraint to some extent, provided the charge transfer at the heterostructure interface is not hampered by their band offsets. Herein, we demonstrate that the intrinsic band offset at the CH3NH3PbI3/MoS2 interface can be overcome by creating sulfur vacancies in MoS2 using a mild plasma treatment; ultrafast hole transfer from CH3NH3PbI3 to MoS2 occurs within 320 fs with 83% efficiency following photoexcitation. Importantly, our work highlights the feasibility of applying defect-engineered 2-D TMDCs as charge-extraction layers in perovskite-based optoelectronic devices.

Sulfur vacancies in monolayer MoS2 and its electrical contacts

The use of reactive electropositive metal contacts is proposed to lower contact resistance in MoS2 devices, based on calculations of the sulfur vacancy in MoS2 by the screened exchange (sX) hybrid functional. sX gives band gaps of 1.88 eV and 1.34 eV for monolayer and bulk MoS2. The S vacancy has a formation energy of 2.35 eV in S-rich conditions, while the Mo vacancy has a large formation energy of 8.02 eV in Mo-rich conditions. The S vacancy introduces defect levels 0/−1 at 1.23 eV and −1/−2 at 1.28 eV in the upper gap. Its formation energy becomes small or negative for EF near the conduction band edge, leading to EF pinning near the conduction band for reactive metal contacts and lower contact resistances.