Oxidation of tantalum disulfide (TaS₂) films for gate dielectric and process design of two-dimensional field-effect device

Ta-based high-κdielectrics can be synthesized via the oxidation of TaS₂films. In this study, we investigated the wet and dry oxidation of TaS₂films via thermal annealing and plasma irradiation, respectively. The specific vibration observed via Raman spectroscopy, the bonding states observed via x-ray photoelectron spectroscopy, and capacitance measurements confirmed the oxidation of TaS₂films with a dielectric constant of ∼14.9. Moreover, the electrical transport of the TaS₂films along the in-plane direction indicated a change in conductivity before and after the oxidation. The thickness of the oxidized film was estimated. Accordingly, the layer-by-layer oxidation was limited to approximately 50 nm via plasma irradiation, whereas the TaS₂films within 150 nm were fully oxidized via thermal annealing in ambient air. Therefore, a Ta-oxide/TaS₂structure was fabricated as a stack material of insulator and metal when the thickness of the pristine film was greater than 50 nm. In addition, Ta-oxide films were integrated into bottom-gated two-dimensional (2D) field-effect transistors (FETs) using the dry transfer method. 2D FETs with multilayer MoTe₂and MoS₂films asp-type andn-type channels, respectively, were successfully fabricated. In particular, the Ta-oxide film synthesized via dry oxidation was used as a gate dielectric, and the device process could be simplified because the Ta-oxide/TaS₂heterostructure can function as a stack material for gate insulators and gate electrodes. An anti-ambipolar transistor consisting of an MoTe₂/MoS₂heterojunction was also fabricated. For the transfer characteristics, a relatively sharp on-state bias range below 10 V and sufficiently high peak-to-valley ratio of 10⁶atV_DS = 3 V were obtained using the high-κ gate dielectric of Ta-oxide despite the presence of the multilayer channels (∼20 nm).