Analysis of femtosecond Raman-induced polarization spectroscopy (RIPS) in N2 and CO2 by fitting and scaling laws

Raman-induced polarization spectroscopy (RIPS) experiments were conducted at room temperature and pressures below 2 atm in pure N2 and CO2. Both homodyne and optically heterodyne detection were used. Calculations of the signal as a function of the pump–probe delay were performed taking into account the pulse duration of the laser, the rotational dependence of the dephasing rates and the small instantaneous electronic Kerr effect. The observed decay and shape of the rotational quantum beats are in good agreement with the calculations. Several sets of linewidth coefficients corresponding to the diagonal part of the collisional–rotational relaxation matrix were used. This matrix was choosen am…