Dual-broadband rotational CARS modelling of nitrogen at pressures up to 9 MPa. I. Inter-branch interference effect

An improved model for pure rotational coherent anti-Stokes Raman scattering (CARS) has been developed or the dual-broadband approach. This model takes into account the fact that coherent anti-Stokes as well as Stokes radiation are generated simultaneously, and these two branches overlap and interact at high pressures giving rise to an inter-branch interference effect. In combustion studies, the anti-Stokes branch is used to determine temperature and concentrations of key species, of which nitrogen is the most widely used, and we have found that the interference effect on the anti-Stokes side is of such magnitude that it clearly needs to be taken into account at pressures of a few MPa. The necessary modifications to the total third-order susceptibility are presented and a derivation of the convolution integral for a finite-bandwidth pump source is given.