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The scalable and conformal synthesis of two-dimensional (2D) transition metal dichalcogenide (TMDC) heterostructures is a persisting challenge for their implementation in next-generation devices. In this work, we report the synthesis of nanometer-thick 2D TMDC heterostructures consisting of TiSx-NbSx on both planar and 3D structures using atomic layer deposition (ALD) at low temperatures (200–300 °C). To this end, a process was developed for the growth of 2D NbSx by thermal ALD using (tert-butylimido)-tris-(diethylamino)-niobium (TBTDEN) and H2S gas. This process complemented the TiSx thermal ALD process for the growth of 2D TiSx-NbSx heterostructures. Precise thickness control of the individual TMDC material layers was demonstrated by fabricating multilayer (5-layer) TiSx-NbSx heterostructures with independently varied layer thicknesses. The heterostructures were successfully deposited on large-area planar substrates as well as over a 3D nanowire array for demonstrating the scalability and conformality of the heterostructure growth process. The current study demonstrates the advantages of ALD for the scalable synthesis of 2D heterostructures conformally over a 3D substrate with precise thickness control of the individual material layers at low temperatures. This makes the application of 2D TMDC heterostructures for nanoelectronics promising in both BEOL and FEOL containing high-aspect-ratio 3D structures. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) heterostructures based on the combination of transition metal dichalcogenides (TMDs) and transition metal oxides (TMOs) have aroused growing attention due to their integrated merits of both components and multiple functionalities. However, nondestructive approaches of constructing TMD-TMO heterostructures are still very limited. Here, we develop a novel type of lateral TMD-TMO heterostructure (NbS2-Nb2O5-NbS2) using a simple lithography-free, direct laser-patterning technique. The perfect contact of an ultrathin TMO channel (Nb2O5) with two metallic TMDs (NbS2) electrodes guarantee strong electrical signals in a two-terminal sensor. Distinct from sensing mechanisms in separate TMOs or TMDs, this sensor works based on the modulation of surface conduction of the ultrathin TMO (Nb2O5) channel through an adsorbed layer of water molecules. The sensor thus exhibits high selectivity and ultrahigh sensitivity for room-temperature detection of NH3 (ΔR/R = 80% at 50 ppm), superior to the reported NH3 sensors based on 2D materials, and a positive temperature coefficient of resistance as high as 15%–20%/°C. Bending-invariant performance and high reliability are also demonstrated in flexible versions of sensors. Our work provides a new strategy of lithography-free processing of novel TMD-TMO heterostructures towards high-performance sensors, showing great potential in the applications of future portable and wearable electronics. [ABSTRACT FROM AUTHOR]

Atomically thin layers of group VB transition metal dichalcogenides (TMDs) provide a unique platform for studying two-dimensional (2D) superconductivity and charge density waves. Thus far, the bottom-up synthesis of these 2D TMDs has often involved precursors that are corrosive or toxic, and their lateral sizes are typically only a few micrometers. In this paper, we report the growth of NbS2 nanoflakes with a thickness down to bilayers and a lateral dimension up to tens of micrometers without using harsh chemical species. NbS2 nanoflakes either standing or lying with respect to the sapphire substrate were obtained by sulfurization of niobium oxide films that were prepared via pulsed laser deposition. Standing nanoflakes are considered to grow epitaxially on the sapphire substrate according to their ordered orientation, while lying nanoflakes with random orientations were grown directly on top of the niobium oxide films. The Raman spectra of the 3R-phase exhibit strong dependence on the layer thickness, where the A1 mode softens as the layer number decreases. In contrast to the stable bulk NbS2, the ultra-thin nanoflakes were oxidized on their top surfaces after prolonged exposure to air, as revealed by X-ray photoelectron spectroscopy. Our work explores an important route to synthesize large-size NbS2 nanoflakes and studies the oxidation process, which is a critical factor to consider if practical applications should be realized in the future. [ABSTRACT FROM AUTHOR]