Polarized Raman spectra obtained from carefully characterized single c
rystals of ZnIn2S4, Zn2In2S5, and Zn3In2S6 are reported. The low-frequ
ency Raman spectra clearly differentiate between the compounds, wherea
s at high frequencies the vibrational features are less sensitive to t
he actual crystal structure. The results are interpreted on the basis
of a molecular-like picture based on the intrinsic cationic disorder.