The state space model of vibrational energy flow: An experimental test using SEP spectra of jet-cooled thiophosgene

Nearly a 1000 X ∼ ← B ∼ transitions of jet-cooled SCCl2 have been measured by stimulated emission pumping. The observed rovibrational band contours cover the 210–330 THz region. A statistical autocorrelation analysis of the spectra answers a key question about the state space model of vibrational energy flow: is the dilution factor σ, which describes how many eigenstates participate in an optically ‘bright’ state due to anharmonic mixing, distributed according to a bimodal probability distribution P(σ) or not? Our SEP data supports a bimodal distribution predicted by state space models.