Observing the ultrafast buildup of a Fano resonance in the time domain.

Although the time-dependent buildup of asymmetric Fano line shapes in absorption spectra has been of great theoretical interest in the past decade, experimental verification of the predictions has been elusive. Here, we report the experimental observation of the emergence of a Fano resonance in the prototype system of helium by interrupting the autoionization process of a correlated two-electron excited state with a strong laser field. The tunable temporal gate between excitation and termination of the resonance allows us to follow the formation of a Fano line shape in time. The agreement with ab initio calculations validates our experimental time-gating technique for addressing an even broader range of topics, such as the emergence of electron correlation, the onset of electron-internuclear coupling, and quasi-particle formation.

Delay in photoemission.

Photoemission from atoms is assumed to occur instantly in response to incident radiation and provides the basis for setting the zero of time in clocking atomic-scale electron motion. We used attosecond metrology to reveal a delay of 21 +/- 5 attoseconds in the emission of electrons liberated from the 2p orbitals of neon atoms with respect to those released from the 2s orbital by the same 100-electron volt light pulse. Small differences in the timing of photoemission from different quantum states provide a probe for modeling many-electron dynamics. Theoretical models refined with the help of attosecond timing metrology may provide insight into electron correlations and allow the setting of the zero of time in atomic-scale chronoscopy with a precision of a few attoseconds.

Probing electron correlation via attosecond xuv pulses in the two-photon double ionization of helium.

Recent experimental developments of high-intensity, short-pulse extreme ultraviolet light sources are enhancing our ability to study electron-electron correlations. We perform time-dependent calculations to investigate the so-called "sequential" regime (variant Planck's over 2piomega > 54.4 eV) in the two-photon double ionization of helium. We show that attosecond pulses allow us not only to probe but also to induce angular and energy correlations of the emitted electrons. The final momentum distribution reveals regions dominated by the Wannier ridge breakup scenario and by postcollision interaction.