Route to Attosecond Nonlinear Spectroscopy

We demonstrate generation of coherent microjoule-scale, low-order harmonic supercontinua in the deep and vacuum ultraviolet (4-9 eV), resulting from the nonlinear transformations of near-single-cycle laser pulses in a gas cell. We show theoretically that their formation is connected to a novel nonlinear regime, holding promise for the generation of powerful deep-UV and vacuum ultraviolet subfemtosecond pulses. Our work opens the route to pump-probe spectroscopy of subfemtosecond-scale valence-shell phenomena in atoms, molecules, and condensed matter.