Reversible Electrochemical Phase Change in Monolayer to Bulk MoTe2 by Ionic Liquid Gating

Abstract

Transition metal dichalcogenides (TMDs) exist in various crystal structures with semiconducting, semi-metallic, and metallic properties. The dynamic control of these phases is of immediate interest for next generation electronics such as phase change memories. Of the binary Mo and W-based TMDs, MoTe2 is attractive for electronic applications because it has the lowest energy difference (40 meV) between the semiconducting (2H) and semi-metallic (1T') phases, allowing for MoTe2 phase change by electrostatic doping. Here we report phase change between the 2H and 1T' polymorphs of MoTe2 in thicknesses ranging from the monolayer case to effective bulk (73nm) using an ionic liquid electrolyte at room temperature and in air. We find consistent evidence of a partially reversible 2H-1T' transition using in-situ Raman spectroscopy where the phase change occurs in the top-most layers of the MoTe2 flake. We find a thickness-dependent transition voltage where higher voltages are necessary to drive the phase change for thicker flakes. We also show evidence of electrochemical activity during the gating process by observation of Te metal deposition. This finding suggests the formation of Te vacancies which have been reported to lower the energy difference between the 2H and 1T' phase, potentially aiding the phase change process. Our discovery that the phase change can be achieved on the surface layer of bulk materials reveals that this electrochemical mechanism does not require isolation of a single layer and the effect may be more broadly applicable than previously thought.

Paper is 15 pages with 7 figures. SI is 13 pages with 8 figures, 2 tables, and 1 video (not uploaded)

References in corpus (4)

• Interference effect on Raman spectrum of graphene on SiO_2/Si
• Strain-Based Room-Temperature Non-Volatile MoTe${}_2$ Ferroelectric Phase Change Transistor
• Double resonance Raman modes in mono- and few-layer MoTe${}_2$
• The role of ionic liquid breakdown in the electrochemical metallization of VO2: An NMR study of gating mechanisms and VO2 reduction

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• Symmetry induced phonon renormalization in few layers of 2H-MoTe${}_2$ transistors: Raman and first-principles studies
• Theoretical study of high harmonic generation in monolayer NbSe${}_2$