Direct determination of state-to-state rotational energy transfer rate constants via a Raman-Raman double resonance technique: ortho-acetylene in v(2)=1 at 155 K

J Chem Phys. 2010 Apr 21;132(15):154303. doi: 10.1063/1.3374031.

Abstract

A new technique for the direct determination of state-to-state rotational energy transfer rate constants in the gas phase is presented. It is based on two sequential stimulated Raman processes: the first one prepares the sample in a single rotational state of an excited vibrational level, and the second one, using the high resolution quasi-continuous stimulated Raman-loss technique, monitors the transfer of population to other rotational states of the same vibrational level as a function of the delay between the pump and the probe stages. The technique is applied to the odd-J rotational states of v(2)=1 acetylene at 155 K. The experimental layout, data acquisition, retrieval procedures, and numerical treatment are described. The quantity and quality of the data are high enough to allow a direct determination of the state-to-state rate constant matrix from a fit of the experimental data, with the only conditions of detailed balance and of a closed number of states. The matrix obtained from this direct fit is also compared with those obtained using some common fitting and scaling laws.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Acetylene / chemistry*
  • Algorithms
  • Energy Transfer*
  • Fluorescence Resonance Energy Transfer / instrumentation
  • Fluorescence Resonance Energy Transfer / methods*
  • Rotation*
  • Temperature*

Substances

  • Acetylene