A series of Mo_xW_{1-x}S₂ (0 ≤ x ≤1) layered mixed crystals was grown by the chemical vapor transport method. A systematic study of these crystals was then conducted using the Raman scattering measurements. The peaks of the two dominant first-order Raman-active modes, A_{1g} and E¹_{2g}, and of several second-order bands are observed from 150 cm¯¹ to 500 cm¯¹. The peaks corresponding to A_{1g} mode show one-mode type behavior, whereas the peaks of E¹_{2g} mode demonstrate two-mode type behavior for the entire series. These results can be explained by the atomic displacements of each mode. For A_{1g} mode, only S atoms vibrate, thereby resulting in a one-mode type behavior for the mixed crystals. For E¹_{2g} mode, metal and S atoms vibrate. The mass difference in the vibrating Mo and W cations causes the two-mode type behavior of E¹_{2g} mode. In addition, the largest asymmetry and broadening of A_{1g} mode for Mo_{0.5}W_{0.5}S₂ is attributed to random alloy scattering.
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