Nonlinear optical response in molecular nitrogen: from ab-initio calculations to optical pulse simulations.

Using first-principle multi-electron calculations via the hybrid anti-symmetrized coupled channels method, we create a model to describe both the nonlinear polarization and ionization of the nitrogen molecule. Based on the metastable electronic state approach, it is designed for space-and-time-resolved simulations in nonlinear optics that require modeling of optical pulses that exhibit rich spectral dynamics and propagate over long distances. As a demonstration of the model's utility, we study low-order harmonic generation in mid-infrared optical filaments.