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We present the first fully ab initio calculations for attosecond transientabsorption spectroscopy of atomic krypton with overlapping pump and probepulses. Within the time-dependent configuration interaction singles (TDCIS)approach, we describe the pump step (strong-field ionization using anear-infrared pulse) as well as the probe step (resonant electron excitationusing an extreme- ultraviolet pulse) from first principles. We extent our TDCISmodel and account for the spin-orbit splitting of the occupied orbitals. Wediscuss the spectral features seen in a recent attosecond transient absorptionexperiment [A. Wirth et al., Science 334, 195 (2011)]. Our results support theconcept that the transient absorption signal can be directly related to theinstantaneous hole population even during the ionizing pump pulse. Furthermore,we find strong deformations in the absorption lines when the overlap of pumpand probe pulses is maximum. These deformations can be described by relativephase shifts in the oscillating ionic dipole. We discuss possible mechanismscontributing to these phase shifts. Our finding suggests that thenon-perturbative laser dressing of the entire N -electron wave function is themain contributor.

Theory of Attosecond Transient Absorption Spectroscopy of Krypton for Overlapping Pump and Probe Pulses