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

Abstract

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.