Anomalous Lattice Dynamics of Mono-, Bi-, and Tri-layer WTe2

Abstract: Tungsten ditelluride (WTe2) is a layered material that exhibits excellent magnetoresistance and thermoelectric behaviors, which are deeply related with its distorted orthorhombic phase that may critically affect the lattice dynamics. Here, for the first time, we present comprehensive characterization of the Raman spectroscopic behavior of WTe2 from bulk to monolayer using experimental and computational methods. We discover that mono and bi-layer WTe2 can be easily identified by Raman spectroscopy since double or single Raman modes that are observed in higher-layer WTe2 are substantially suppressed in the monolayer and bilayer WTe2, respectively. In addition, different from hexagonal metal dichalcogenides, the frequency of in-plane mode of WTe2 remains almost constant as the layer number decreases, while the other Raman modes consistently blueshift. First-principles calculation validates the experiments and reveals that the negligible shift of the mode is attributed to the lattice vibration along the tungsten chains that make WTe2 structurally one-dimensional.