Molecular dynamics in the solid state: Mössbauer and Raman spectroscopy of (CH3)2SN(C5H7O2)2

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Abstract
The 119Sn Mössbauer effect resonance has been measured for dimethyltin(IV) bis acetylacetonate over the temperature range 4.2≤T≤120°K, and isomer shift, quadrupole splitting, recoil‐free fraction, and Gol'danskii‐Karyagin asymmetry parameters have been obtained over this interval. The resultant values for fa and the asymmetry parameter have been compared with the corresponding room temperature data extracted from x‐ray diffraction results and permit a detailed evaluation of the vibrational motion of the metal atom in this quasioctahedral compound. On the basis of the temperature dependence of fa, it is possible to assign the Raman active mode observed at 37 cm−1 for the neat solid to an intra‐unit‐cell vibration of the two molecules against each other, confirming the essentially monomeric nature of the solid in the covalent lattice. Results of Mössbauer experiments on frozen solutions of this compound in glassy matrices lead to the conclusion that major structural differences exist between the neat solid (as probed by x‐ray diffraction) and the molecule in solution (as probed by dipole moment measurements) and suggest that the structural inferences drawn by earlier investigators may not be mutually inconsistent.