Coherent light pulses of few to hundreds of femtoseconds (fs) duration have prolifically served the field of ultrafast phenomena. While fs pulses address mainly dynamics of nuclear motion in molecules or lattices in the gas, liquid or condensed matte
r phase, the advent of attosecond pulses has in recent years provided direct experimental access to ultrafast electron dynamics. However, there are processes involving nuclear motion in molecules and in particular coupled electronic and nuclear motion that possess few fs or even sub-fs dynamics. In the present work we have succeeded in addressing simultaneously vibrational and electronic dynamics in molecular Hydrogen. Utilizing a broadband extreme-ultraviolet (XUV) continuum the entire, Frank-Condon allowed spectrum of H2 is coherently excited. Vibrational, electronic and ionization 1fs scale dynamics are subsequently tracked by means of XUV-pump-XUV-probe measurements. These reflect the intrinsic molecular behavior as the XUV probe pulse hardly distorts the molecular potential.
Studies of ultrafast dynamics along with femtosecond-pulse metrology rely on non-linear processes, induced solely by the exciting/probing pulses or the pulses to be characterized. Extension of these approaches to the extreme-ultraviolet (XUV) spectra
l region opens up a new, direct route to attosecond scale dynamics. Limitations in available intensities of coherent XUV continua kept this prospect barren. The present work overcomes this barrier. Reaching condition at which simultaneous ejection of two bound electrons by two-XUV-photon absorption becomes more efficient than their one-by-one removal it is succeeded to probe atomic coherences, evolving at the 1fs scale, and determine the XUV-pulse duration. The investigated rich and dense in structure autoionizing manifold ascertains applicability of the approach to complex systems. This initiates the era of XUV-pump-XUV-probe experiments with attosecond resolution.
