Quantum coherent control of the photo\-electron angular distribution in bichromatic ionization of atomic neon

We investigate the coherent control of the photo\-electron angular distribution in bichromatic atomic ionization. Neon is selected as target since it is one of the most popular systems in current gas-phase experiments with free-electron lasers (FELSs). In particular, we tackle practical questions, such as the role of the fine-structure splitting, the pulse length, and the intensity. Time-dependent and stationary perturbation theory are employed, and we also solve the time-dependent Schr\"odinger equation in a single-active electron model. We consider neon ionized by a FEL pulse whose fundamental frequency is in resonance with either $2p-3s$ or $2p-4s$ excitation. The contribution of the non\-resonant two-photon process and its potential constructive or destructive role for quantum coherent control is investigated.Comment: 10 pages, 6 figure

Interfering one-photon and two-photon ionization by femtosecond VUV pulses in the region of an intermediate resonance

The electron angular distribution after atomic photoionization by the fundamental frequency and its second harmonic is analyzed for a case when the frequency of the fundamental scans the region of an intermediate atomic state. The angular distribution and its left-right asymmetry, due to the two-pathway interference between nonresonant one-photon and resonant two-photon ionization, sharply change as a function of the photon energy. The phenomenon is exemplified by both solving the time-dependent Schr\"odinger equation on a numerical space-time grid and by applying perturbation theory for ionization of the hydrogen atom in the region of the 1s\text{\ensuremath{-}}2p transition for femtosecond pulses as well as an infinitely long exposure to the radiation. Parametrizations for the asymmetry and the anisotropy coefficients, obtained within perturbation theory, reveal general characteristics of observable quantities as functions of the parameters of the radiation beam

Analysis of two-color photoelectron spectroscopy for attosecond metrology at seeded free-electron lasers

The generation of attosecond pulse trains at free-electron lasers opens new opportunities in ultrafast science, as it gives access, for the first time, to reproducible, programmable, extreme ultraviolet (XUV) waveforms with high intensity. In this work, we present a detailed analysis of the theoretical model underlying the temporal characterization of the attosecond pulse trains recently generated at the free-electron laser FERMI. In particular, the validity of the approximations used for the correlated analysis of the photoelectron spectra generated in the two-color photoionization experiments are thoroughly discussed. The ranges of validity of the assumptions, in connection with the main experimental parameters, are derived

Coherent control with a short-wavelength free-electron laser

Extreme ultraviolet and X-ray free-electron lasers (FELs) produce short-wavelength pulses with high intensity, ultrashort duration, well-defined polarization and transverse coherence, and have been utilized for many experiments previously possible only at long wavelengths: multiphoton ionization, pumping an atomic laser and four-wave mixing spectroscopy. However one important optical technique, coherent control, has not yet been demonstrated, because self-amplified spontaneous emission FELs have limited longitudinal coherence. Single-colour pulses from the FERMI seeded FEL are longitudinally coherent, and two-colour emission is predicted to be coherent. Here, we demonstrate the phase correlation of two colours, and manipulate it to control an experiment. Light of wavelengths 63.0 and 31.5nm ionized neon, and we controlled the asymmetry of the photoelectron angular distribution by adjusting the phase, with a temporal resolution of 3as. This opens the door to new short-wavelength coherent control experiments with ultrahigh time resolution and chemical sensitivity

Non-dipole effects in the angular distribution of photoelectrons in sequential two-photon atomic double ionization

Motivated by the recent achievements of experiments using x-ray free electron lasers, we have developed a theory for the angular distributions of photoelectrons in sequential two-photon double ionization (2PDI) of atoms beyond the dipole approximation. Expressions for the angular distributions are obtained taking into account the full multipole expansion of radiation in electric and magnetic moments. The formalism is further specified for the first-order corrections to the dipole approximation. As an illustrative example, the sequential 2PDI of the 2p shell in atomic neon is studied. The numerical calculations predict distinct non-dipole effects observable in experiments at present x-ray free electron lasers

Non-dipole effects in the angular distribution of photoelectrons in sequential two-photon double ionization: argon and neon

As an extension to recent developments in the theory of non-dipole effects in nonlinear photoprocesses in the XUV/x-ray wavelength regime, the sequential two-photon double ionization of the 3p shell in atomic argon is studied theoretically and compared to similar processes in the 2p shell of neon. The calculations predict distinct non-dipole effects in the region of the Cooper minimum in argon at photon energies around 50 eV, where they are of similar importance as at photon energies of more than 500 eV. The non-dipole effects should therefore be clearly observable in experiments performed at the present x-ray free electron lasers