On the relative roles of higher-order nonlinearity and ionization in ultrafast light-matter interactions.

Far off-resonant ultrafast and nonlinear light-matter interactions are studied using a one-dimensional atomic model. Results from a pump-probe diagnostic reveal that any higher-order nonlinear refraction is masked by ionization-induced defocusing before it becomes significant. On the other hand, we show that signatures of a higher-order nonlinearity may still be manifest via low-order harmonics of the pump center frequency. Implications for filamentation of femtosecond pulses are pointed out.