Abstract
The Raman and infrared spectra of crystalline CS2 have been observed at low temperatures. The Raman band 2ν2 and the infrared band ν3 have been found to split into two components, while no splitting has been seen for the Raman band ν1. That the rule of mutual exclusion holds for the Raman and infrared spectra of crystalline CS2 indicates the inversion symmetry of the molecule is preserved even in the crystal. A dipole—dipole coupling model for the intermolecular interactions in the crystal explains the band splitting. Two low‐frequency Raman bands have been observed and assigned to the lattice vibrations of rotational mode.