The synthesis of atomically thin transition-metal disulfides (MS2) with layer controllability and large-area uniformity is an essential requirement for their application in electronic and optical devices. In this work, we describe a process for the synthesis of WS2 nanosheets through the sulfurization of an atomic layer deposition (ALD) WO3 film with systematic layer controllability and wafer-level uniformity. The X-ray photoemission spectroscopy, Raman, and photoluminescence measurements exhibit that the ALD-based WS2 nanosheets have good stoichiometry, clear Raman shift, and bandgap dependence as a function of the number of layers. The electron mobility of the monolayer WS2 measured using a field-effect transistor (FET) with a high-k dielectric gate insulator is shown to be better than that of CVD-grown WS2, and the subthreshold swing is comparable to that of an exfoliated MoS2 FET device. Moreover, by utilizing the high conformality of the ALD process, we have developed a process for the fabrication of WS2 nanotubes.

The effective synthesis of two-dimensional transition metal dichalcogenides alloy is essential for successful application in electronic and optical devices based on a tunable band gap. Here we show a synthesis process for Mo1−xWxS2 alloy using sulfurization of super-cycle atomic layer deposition Mo1−xWxOy. Various spectroscopic and microscopic results indicate that the synthesized Mo1−xWxS2 alloys have complete mixing of Mo and W atoms and tunable band gap by systematically controlled composition and layer number. Based on this, we synthesize a vertically composition-controlled (VCC) Mo1−xWxS2 multilayer using five continuous super-cycles with different cycle ratios for each super-cycle. Angle-resolved X-ray photoemission spectroscopy, Raman and ultraviolet–visible spectrophotometer results reveal that a VCC Mo1−xWxS2 multilayer has different vertical composition and broadband light absorption with strong interlayer coupling within a VCC Mo1−xWxS2 multilayer. Further, we demonstrate that a VCC Mo1−xWxS2 multilayer photodetector generates three to four times greater photocurrent than MoS2- and WS2-based devices, owing to the broadband light absorption.

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The characteristics of the atomic layer deposition (ALD) of SrTiO3 (STO) films were examined for metal–insulator–metal capacitors, with Cp-based precursors Sr(iPr3Cp)2 and Cp*Ti(OMe)3 [Cp* = C5(CH3)5] employed as the Sr and Ti precursors, respectively. While the Sr precursor has a higher reactivity toward oxygen on the Ru substrate compared with another Ti precursor, with a 2,2,6,6-tetramethyl-3,5-heptanedionato ligand, which results in the highly Sr excessive STO film, the enhanced reactivity of the present Ti precursor suppressed the unwanted excessive incorporation of Sr into the film. A possible mechanism for the Sr overgrowth and retardation is suggested in detail. By controlling the subcycle ratio of SrO and TiO2 layers, stoichiometric STO could be obtained, even without employing a deleterious reaction barrier layer. This improved the attainable minimum equivalent oxide thickness of the Pt/STO/RuO2 capacitor to 0.43 nm, with acceptable leakage current density (∼8 × 10–8 A/cm2). This indicates an improvement of ∼25% in the capacitance density compared with previous work.