期刊
ACS NANO
卷 13, 期 4, 页码 3896-3909出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.8b06515
关键词
WS2 and WO3-x suboxides; transition-metal dichalcogenides; two-dimensional layered materials; nanotubes; chemical vapor deposition growth; linear and nonlinear optical properties; second harmonic generation
类别
资金
- University of Bath
- Royal Society [CHG\R1\170067, PEF1\170015, RGF\EA\180228]
- STFC [ST/R005842/1]
- Engineering and Physical Sciences Research Council, UK, via the Centre for Doctoral Training in Condensed Matter Physics (CDTCMP) [EP/L015544/1]
We demonstrate a versatile, catalyst free chemical vapor deposition process on insulating substrates capable of producing in one single stream one-dimensional (1D) WO3-x suboxides leading to a wide range of substrate-supported 2H-WS2 polymorphs: a tunable class of out-of-plane (of the substrate) nanophases, with 1D nanotubes and a pure WS2, two-dimensional (2D) nano mesh (defined as a network of webbed, micron-size, few layer 2D sheets) at its extremes; and in-plane (parallel to the substrate) mono- and few-layer 2D domains. This entails a two-stage approach in which the 2WO(3) + 7S -> 2WS(2) + 3SO(2) reaction is intentionally decoupled. First, various morphologies of nanowires or nanorods of high stoichiometry, WO2.92/WO2.9 suboxides (belonging to the class of Magnai phases) were formed, followed by their sulfurization to undergo reduction to the aforementioned WS2 polymorphs. The continuous transition of WS2 from nanotubes to the out-of-plane 2D nanomesh, via intermediary, mixed 1D-2D phases, delivers tunable functional properties, for example, linear and nonlinear optical properties, such as reflectivity (linked to optical excitations in the material), and second harmonic generation (SHG) and onset of saturable absorption. The SHG effect is very strong across the entire tunable class of WS2 nanomaterials, weakest in nanotubes, and strongest in the 2D nanomesh. Furthermore, a mechanism via suboxide (WO3-x) intermediate as a possible path to 2D domain growth is demonstrated. 2D, in-plane WS2 domains grow via self-seeding and feeding where short WO2.92/WO2.9 nanorods provide both the nucleation sites and the precursor feedstock. Understanding the reaction path (here, in the W-O-S space) is an emerging approach toward controlling the nucleation, growth, and morphology of 2D domains and films of transition-metal dichalcogenides.
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