High resolution femtosecond coherent anti-Stokes Raman scattering: Determination of rotational constants, molecular anharmonicity, collisional line shifts, and temperature

Abstract

In this paper we present high resolution spectroscopy performed with femtosecond coherent anti-Stokes Raman scattering (CARS). After a theoretical treatment of the issue, specific experimental configurations will be introduced. Transients from nonresonant rotational and vibrational CARS on di- and polyatomics in the gas phase were analyzed. Rotational and vibrational constants and pressure-dependent line shifts are determined with high accuracy. The method is suitable for precise measurement of temperatures. We present thermometry on combustion relevant species like H2 and N2 and discuss the reliability and accuracy of the data.