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Atmospheric lasing has aroused much interest in the past few years. The 'air–laser' opens promising potential for remote chemical sensing of trace gases with high sensitivity and specificity. At present, several approaches have been successfully implemented for generating highly coherent laser beams in atmospheric condition, including both amplified-spontaneous emission, and narrow-bandwidth stimulated emission in the forward direction in the presence of self-generated or externally injected seed pulses. Here, we report on generation of multiple-wavelength Raman lasers from nitrogen molecular ions (), driven by intense mid-infrared laser fields. Intuitively, the approach appears problematic for the small nonlinear susceptibility of ions, whereas the efficiency of Raman laser can be significantly promoted in near-resonant condition. More surprisingly, a Raman laser consisting of a supercontinuum spanning from ~310 to ~392 nm has been observed resulting from a series near-resonant nonlinear processes including four-wave mixing, stimulated Raman scattering and cross phase modulation. To date, extreme nonlinear optics in molecular ions remains largely unexplored, which provides an alternative means for air–laser-based remote sensing applications.

Generation of Raman lasers from nitrogen molecular ions driven by ultraintense laser fields