Isotopically resolved photoelectron imaging unravels complex atomic autoionization dynamics by two-color resonant ionization.

Angle-resolved electron spectroscopy in coincidence with high-resolution mass spectroscopy has been applied to study two-color resonant photoionization in atomic xenon. Separation of different isotopes enabled us to extract results for the electronic dynamics free from depolarization effects, which are generally introduced by the coupling of the electronic and nuclear angular momenta. The concerted experimental and theoretical analysis of the photoelectron angular distributions in the region of an autoionizing resonance emphasizes the strong sensitivity of the observed structures to the fine details of the treatment of the underlying dynamics.

Symmetry breakdown of electron emission in extreme ultraviolet photoionization of argon.

Short wavelength free-electron lasers (FELs), providing pulses of ultrahigh photon intensity, have revolutionized spectroscopy on ionic targets. Their exceptional photon flux enables multiple photon absorptions within a single femtosecond pulse, which in turn allows for deep insights into the photoionization process itself as well as into evolving ionic states of a target. Here we employ ultraintense pulses from the FEL FERMI to spectroscopically investigate the sequential emission of electrons from gaseous, atomic argon in the neutral as well as the ionic ground state. A pronounced forward-backward symmetry breaking of the angularly resolved emission patterns with respect to the light propagation direction is experimentally observed and theoretically explained for the region of the Cooper minimum, where the asymmetry of electron emission is strongly enhanced. These findings aim to originate a better understanding of the fundamentals of photon momentum transfer in ionic matter.

Polarization control in two-color above-threshold ionization of atomic helium.

Two-color multiphoton ionization of atomic helium was investigated by combining extreme ultraviolet (XUV) radiation from the Free Electron Laser in Hamburg with an intense synchronized optical laser. In the photoelectron spectrum, lines associated with direct ionization and above-threshold ionization show strong variations of their amplitudes as a function of both the intensity of the optical dressing field and the relative orientation of the linear polarization vectors of the two fields. The polarization dependence provides direct insight into the symmetry of the outgoing electrons in above-threshold ionization. In the high field regime, the monochromaticity of the XUV radiation enables the unperturbed observation of nonlinear processes in the optical field.