Anomalous Fano Profiles in External Fields.

We show that the external control of Fano resonances in general leads to complex Fano q parameters. Fano line shapes of photoelectron and transient absorption spectra in the presence of an infrared control field are investigated. Computed transient absorption spectra are compared with a model proposed for a recent experiment [C. Ott et al., Science 340, 716 (2013)]. Control mechanisms for photoelectron spectra are exposed: control pulses applied during excitation modify the line shapes by momentum boosts of the continuum electrons. Pulses arriving after excitation generate interference fringes due to infrared two-photon transitions.

Time-resolved photoemission on the attosecond scale: opportunities and challenges.

The interaction of laser pulses of sub-femtosecond duration with matter opened up the opportunity to explore electronic processes on their natural time scale. One central conceptual question posed by the observation of photoemission in real time is whether the ejection of the photoelectron wavepacket occurs instantaneously, or whether the response time to photoabsorption is finite leading to a time delay in photoemission. Recent experimental progress exploring attosecond streaking and RABBIT techniques find relative time delays between the photoemission from different atomic substates to be of the order of -20 attoseconds. We present ab initio simulations for both one- and two-electron systems which allow the determination of both absolute and relative time delays with -1 attosecond precision. We show that the intrinsic time shift of the photoionization process encoded in the Eisenbud-Wigner-Smith delay time can be unambiguously disentangled from measurement-induced time delays in a pump-probe setting when the photoionized electronic wavepacket is probed by a modestly strong infrared streaking field. We identify distinct contributions due to initial-state polarization, Coulomb-laser coupling in the final continuum state as well as final-state interaction with the entangled residual ionic state. Extensions to multi-electron systems and to the extraction of time information in the presence of decohering processes are discussed.

Attosecond streaking of correlated two-electron transitions in helium.

We present fully ab initio simulations of attosecond streaking for ionization of helium accompanied by shakeup of the second electron. This process represents a prototypical case for strongly correlated electron dynamics on the attosecond time scale. We show that streaking spectroscopy can provide detailed information on the Eisenbud-Wigner-Smith time delay as well as on the infrared-field dressing of both bound and continuum states. We find a novel contribution to the streaking delay that stems from the interplay of electron-electron and infrared-field interactions in the exit channel. We quantify all the contributions with attosecond precision and provide a benchmark for future experiments.