Raman Spectroscopy of Few‐Layers TaS2 and Mo‐Doped TaS2 with Enhanced Superconductivity

The use of simple, fast and economic experimental tools to characterize low-dimensional materials is an important step in the process of democratizing the use of such materials in laboratories around the world. Raman spectroscopy has arisen as a way of indirectly determining the thickness of nanolayers of transition metal dichalcogenides (TMDs), avoiding the use of more expensive tools such as atomic force microscopy, and it is therefore a widely used technique in the study of semiconducting TMDs. However, the study of many metallic TMDs in the limit of few atomic layers is still behind when compared to their semiconducting counterparts, partly due to the lack of similar alternative characterization studies. In this work we present the characterization of the Raman spectrum, specifically of the E$^1_{2g}$- and A$_{1g}$-modes, of mechanically exfoliated crystals of Ta$_{1-x}$Mo$_x$S$_2$, a metallic TMD which exhibits charge density wave formation and superconductivity. The clear identification of contributions to the Raman spectrum coming from the SiO$_2$/Si substrate, which overlap with the peaks coming from the sample, and which dominate in intensity in the few-layer-samples limit, allowed the isolation of the individual E$^1_{2g}$- and A$_{1g}$-modes of the samples and, for the first time, the observation of a clear evolution of the Raman shifts of both modes as a function of sample thickness. The evolution of such peaks qualitatively resembles the evolution seen in other TMDs, and provide a way of indirectly determining sample thickness in the limit of few atomic layers at a low cost. In addition, we observe a softening (red-shift) of both E$^1_{2g}$- and A$_{1g}$-modes with Mo-doping in the nanolayers, possibly related to the increased out-of-plane lattice parameter with respect to the pure compound.