Laser-induced gratings in the gas phase excited by Raman-active transitions

We report on a new time-resolved coherent Raman technique that is based on the generation of thermal gratings following a population change among molecular levels that is induced by stimulated Raman pumping. This is achieved by use of spatially and temporally overlapping intensity interference patterns generated independently by two lasers. When this technique is used in carbon dioxide, making use of transitions that belong to the Q branches of the v(1)/2v Fermi dyad, it is possible to investigate molecular energy transfer processes. A further unique feature of this method is spectral resolution that is better than that achieved by coherent anti-Stokes Raman scattering.