Cybernetic spectroscopy of molecular rototranslation in the liquid state

Abstract

We introduce (following Ciccotti et al.) the subject of cybernetic spectroscopy with reference to the computer simulation of rototranslational mixed a.c.f.'s in the molecule-fixed frame of CH₂Cl₂ in the liquid state (E.M.L.G. pilot project). The detailed acquisition of such “signatures” is possible only via numerical methods using fast computers and provides a corroborative challenge both in the fields of experimental spectroscopy and phenomenological theory. Up to nine elements each of the mixed a.c.f. matrices are observable depending on molecular symmetry. The properties of these elements are basically important in the interpretation of molecular diffusion and broad-band spectroscopy of liquids and mesophases.