High-resolution spectroscopy and analysis of the stretching dyad of osmium tetroxide

Abstract OsO4 is a heavy tetrahedral molecule that may constitute a benchmark for quantum chemistry calculations. Its favorable spin statistics (due to the zero nuclear spin of oxygen atoms) is such that only A1 and A2 rovibrational levels are allowed, leading to a dense, but quite easily resolved spectrum. Most lines are single ones, instead of complex line clusters as in the case of other heavy spherical-tops like SF6, for instance. It is thus possible to fully assign and fit the spectrum and to obtain precise experimental effective molecular parameters. The strong ν 3 stretching fundamental has been studied a long time ago as an isolated band [McDowell RS, Radziemski LJ, Flicker H, Galbr…