Atomically thin MoS2 crystals have been recognized as a quasi-2D semiconductor with remarkable physical properties. This letter reports our Raman scattering measurements on multilayer and monolayer MoS2, especially in the low-frequency range (<50 cm −1 ). We find two low-frequency Raman modes with contrasting thickness dependence. With increasing the number of MoS2 layers, one shows a significant increase in frequency while the other decreases following a 1/N (N denotes the number of unit layers) trend. With the aid of first-principles calculations we assign the former as the shear mode E 2 2g . The latter is distinguished as the compression vibrational mode, similar to the surface vibration of other epitaxial thin films. The opposite evolution of the two modes with thickness demonstrates novel vibrational modes in atomically thin crystal as well as a new and more precise way to characterize thickness of atomically thin MoS2 films. In addition, we observe a broad feature around 38 cm −1 ( 5 meV) which is visible only under near-resonance excitation and pinned at the fixed energy independent of thickness. We interpret the feature as an electronic Raman scattering associated with the spin-orbit coupling induced splitting in conduction band at K points in their Brillouin zone.

We report a dramatic change in the intensity of a Raman mode with applied magnetic field, displaying a gigantic magnetooptical effect. Using the nonmagnetic layered material MoS 2 as a prototype system, we demonstrate that the application of a magnetic field perpendicular to the layers produces a dramatic change in intensity for the out-of-plane vibrations of S atoms, but no change for the in-plane breathing mode. The distinct intensity variation between these two modes results from the effect of field-induced broken symmetry on Raman scattering cross-section. A quantitative analysis on the field-dependent integrated Raman intensity provides a unique method to precisely determine optical mobility. Our analysis is symmetry-based and material-independent, and thus the observations should be general and inspire a new branch of inelastic light scattering and magneto-optical applications.Raman | layered | magneto-optical | broken symmetry | phonon

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