Engineering the Structural and Electronic Phases of MoTe2 through W Substitution

Abstract

MoTe₂ is an exfoliable transition metal dichalcogenide (TMD) that crystallizes in three symmetries: the semiconducting trigonal-prismatic 2H- or α-phase, the semimetallic and monoclinic 1T^'- or β-phase, and the semimetallic orthorhombic γ-structure. The 2H-phase displays a band gap of ∼1 eV making it appealing for flexible and transparent optoelectronics. The γ-phase is predicted to possess unique topological properties that might lead to topologically protected nondissipative transport channels. Recently, it was argued that it is possible to locally induce phase-transformations in TMDs, through chemical doping, local heating, or electric-field to achieve ohmic contacts or to induce useful functionalities such as electronic phase-change memory elements. The combination of semiconducting and topological elements based upon the same compound might produce a new generation of high performance, low dissipation optoelectronic elements. Here, we show that it is possible to engineer the phases of MoTe₂ through W substitution by unveiling the phase-diagram of the Mo_1-xW_xTe₂ solid solution, which displays a semiconducting to semimetallic transition as a function of x. We find that a small critical W concentration x_c ∼ 8% stabilizes the γ-phase at room temperature. This suggests that crystals with x close to x_c might be particularly susceptible to phase transformations induced by an external perturbation, for example, an electric field. Photoemission spectroscopy, indicates that the γ-phase possesses a Fermi surface akin to that of WTe₂.

Keywords: Raman spectroscopy; Transition-metal-dichalcogenides; Weyl semimetals; electron microscopy; phase-transformations; photoemission spectroscopy.