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

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 (IT') phases, allowing for MoTe2 phase change by electrostatic doping. Here, we report phase change between the 2H and IT' polymorphs of MoTe2 in thicknesses ranging from the monolayer to bulk-like case (73 nm) using an ionic liquid electrolyte at room temperature and in air. We find consistent evidence of a partially reversible 2H-IT' transition using in situ Raman spectroscopy where the phase change occurs in the topmost 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 formation. This finding suggests the formation of Te vacancies which have been reported to lower the energy difference between the 2H and IT' phases, potentially aiding the phase change process. Our discovery that the phase change can be achieved on the surface layer of bulk-like 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.