Relativistic Two-Photon Matrix Elements for Attosecond Delays

Abstract

The theory of one-photon ionization and two-photon above-threshold ionization is formulated for applications to heavy atoms in attosecond science by using Dirac–Fock formalism. A direct comparison of Wigner–Smith–Eisenbud delays for photoionization is made with delays from the Reconstruction of Attosecond Beating By Interference of Two-photon Transitions (RABBIT) method. Photoionization by an attosecond pulse train, consisting of monochromatic fields in the extreme ultraviolet range, is computed with many-body effects at the level of the relativistic random phase approximation (RRPA). Subsequent absorption and emission processes of infrared laser photons in RABBIT are evaluated by using static ionic potentials as well as asymptotic properties of relativistic Coulomb functions. As expected, light elements, such as argon, show negligible relativistic effects, whereas heavier elements, such a krypton and xenon, exhibit delays that depend on the fine-structure of the ionic target. The relativistic effects are notably close to ionization thresholds and Cooper minima with differences in fine-structure delays predicted to be as large as tens of attoseconds. The separability of relativistic RABBIT delays into a Wigner–Smith–Eisenbud delay and a universal continuum–continuum delay is studied with reasonable separability found for photoelectrons emitted along the laser polarization axis in agreement with prior non-relativistic results.