Dramatic Spectral Broadening of Ultrafast Laser Pulses in Molecular Nitrogen Ions

We investigate nonlinear interaction of nitrogen molecules with a two-color laser field composed by an intense 800 nm laser pulse and a weak 400 nm laser pulse. It is demonstrated that the spectrum of 400 nm pulses is dramatically broadened when the two beams temporally overlap. In comparison, the spectral broadening in argon is less pronounced, although argon atoms and nitrogen molecules have comparable ionization potentials. We reveal that the dramatic spectral broadening originates from the greatly enhanced nonlinear optical effects in the near-resonant condition of interaction between the 400 nm pulses and the nitrogen molecular ions.