In a seminal article, Fano predicts that absorption of light occurs preferably with increase of angular momentum. Here we generalize Fano's propensity rule to laser-assisted photoionization, consisting of absorption of an extreme-ultraviolet photon followed by absorption or emission of an infrared photon. The predicted asymmetry between absorption and emission leads to incomplete quantum interference in attosecond photoelectron interferometry. It explains both the angular-dependence of the photoionization time delays and the delay-dependence of the photoelectron angular distributions. Our theory is verified by experimental results in Ar in the 20-40 eV range.
We present calculations for attosecond atomic delays in photoionization of noble gas atoms based on full two-color two-photon Random-Phase Approximation with Exchange in both length and velocity gauge. Gauge invariant atomic delays are demonstrated for the complete set of diagrams. The results are used to investigate the validity of the common assumption that the measured atomic delays can be interpreted as a one-photon Wigner delay and a universal continuum-continuum contribution that depends only on the kinetic energy of the photoelectron, the laser frequency and the charge of the remaining ion, but not on the specific atom or the orbital from which the electron is ionized. Here we find that although effects beyond the universal IR-photoelectron continuumcontinuum transitions are rare, they do occur in special cases such as around the 3s Cooper minimum in argon. We conclude also that in general the convergence in terms of many-body diagrams is considerably faster in length gauge than in velocity gauge.
The photoionization of xenon atoms in the 70–100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe+ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as, and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide insight into the complex electron-spin dynamics of photo-induced phenomena.
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