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Atomically thin MoS$_{2}$ crystals have been recognized as a quasi-2Dsemiconductor with remarkable physics properties. This letter reports our Ramanscattering measurements on multilayer and monolayer MoS$_{2}$, especially inthe low-frequency range ($<$50 cm$^{-1}$). We find two low-frequency Ramanmodes with contrasting thickness dependence. With increasing the number ofMoS$_{2}$ layers, one shows a significant increase in frequency while the otherdecreases following a 1/N (N denotes layer-number) trend. With the aid offirst-principle calculations we assign the former as the shear mode$E_{2g}^{2}$ and the latter as the compression vibrational mode. The oppositeevolution of the two modes with thickness demonstrates novel vibrational modesin atomically thin crystal as well as a new and more precise way tocharacterize thickness of atomically thin MoS$_{2}$ films. In addition, weobserve a broad feature around 38 cm$^{-1}$ (~5 meV) which is visible onlyunder near-resonance excitation and pinned at the fixed energy independent ofthickness. We interpret the feature as an electronic Raman scatteringassociated with the spin-orbit coupling induced splitting in conduction band atK points in their Brillouin zone.

Low-Frequency Raman Modes and Electronic Excitations In Atomically Thin MoS2 Crystals