Ultra‐Broadband Visible‐DUV Supercontinuum Generation by Non‐Resonant Coherent Raman Scattering in Air

To date, supercontinuum light in the visible and near‐infrared ranges is readily realizable by the optical Kerr effect through self‐phase modulation of ultrashort laser pulses in transparent media. However, it is still a challenge to extend the supercontinuum spectrum down to the deep‐ultraviolet (DUV) range, which is particularly needed for exploring ultrafast dynamics in chemistry, materials, and biology. Here, an approach of non‐resonant coherent Raman scattering is developed to generate ultra‐broadband visible‐DUV supercontinuum in ambient air with a spectral range spanning over 250 nm and a wavelength down to 220 nm. A rovibrational coherence is established in air molecules by filamentation of a near‐infrared femtosecond 800 nm pulse and two femtosecond Raman laser pulses at 267 and 400 nm are introduced into the coherent media to induce non‐resonant coherent Stokes and anti‐Stokes Raman scatterings, which serve as the spectral bridges to link the neighboring Raman pump laser spectra, resulting in ultra‐broadband supercontinuum light. The mechanism is further verified by examining the broadening of picosecond N2+ laser lines with narrow bandwidths (10–30 cm−1), which forms a supercontinuum spectrum spanning over 150 nm. The work provides a viable route for the establishment of coherent DUV supercontinuum in the gas media at designed wavelength ranges.