Abstract
The spontaneous Raman spectra of the ν1 band of SiD4 in the liquid and plastic crystalline phases have been modeled by a memory‐function procedure. It was found to be necessary to go to third order in the memory‐function procedure. In order to get agreement between the ν2 reorientational relaxation times and the deuteron magnetic resonance correlation times, anisotropic rotation has been postulated. The anisotropic rotation accounts for an additional slow variable in the vibrational dephasing dynamics. The ν1 vibration is apparently modulated by the rotations. The vibrational–correlation function is reported out to 10 ps.