The ratios of photoionization cross sections of the 1σg and 1σu shells of the N2 molecule for the vibrational transitions to the v′ = 0 and v′ = 1 core-ionized states in the photon energy region between 440 and 550 eV have been measured. The calculations in the random phase approximation well reproduce the experimental data. The variation of the ratio with photon energy is attributed to the interference modulation that is caused by coherent photoemission from the two atoms, as an analogue of the Young's double-slit experiment. The calculations extended up to 1.8 keV allow connecting the modulation with the onset of transitions to the states of increasing orbital angular momentum which occurs at increasing photon energies and demonstrate that the main contribution to these modulations comes from the σ continuum states.

We have measured the vibrational structures of the N 1s photoelectron mainline and satellites of the gaseous N2 molecule with the resolution better than 75 meV. The gerade and ungerade symmetries of the core-ionized (mainline) states are resolved energetically, and symmetry-dependent angular distributions for the satellite emission allow us to resolve the Sigma and Pi symmetries of the shake-up (satellite) states. Symmetry-adapted cluster-expansion configuration-interaction calculations of the potential energy curves for the mainline and satellite states along with a Franck-Condon analysis well reproduce the observed vibrational excitation of the bands, illustrating that the theoretical calculations well predict the symmetry-dependent geometry relaxation effects. The energies of both mainline states and satellite states, as well as the splitting between the mainline gerade and ungerade states, are also well reproduced by the calculation: the splitting between the satellite gerade and ungerade states is calculated to be smaller than the experimental detection limit.

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We have measured the vibrationally resolved partial cross sections σ v 1 and asymmetry parameters β v 1 for C K-shell photoionization of the CO 2 molecule in the u shape resonance region above the C K-shell ionization threshold. The positions of both the maxima of σ v 1 and the minima of β v 1 move towards the C K-shell threshold with increasing symmetric stretching vibrational excitation v 1 in the C 1s single-hole state. Calculations employing the relaxed-core Hartree-Fock approach reproduce the observed vibrational effects.

A low-temperature discharge nozzle source with a liquid-N(2) circulator for He*(2(3)S) metastable atoms has been developed in order to obtain the state-resolved collision energy dependence of Penning ionization cross sections in a low collision energy range from 20 to 80 meV. By controlling the discharge condition, we have made it possible to measure the collision energy dependence of partial ionization cross sections (CEDPICS) for a well-studied system of CH(3)CN+He*(2(3)S) in a wide energy range from 20 to 350 meV. The anisotropic interaction potential energy surface for the present system was obtained starting from an ab initio model potential via an optimization procedure based on classical trajectory calculations for the observed CEDPICS. A dominant attractive well depth was found to be 423 meV (ca. 10 kcal/mol) at a distance of 3.20 A from the center of mass of CH(3)CN in the N-atom side along the CCN axis. In addition, a weak attractive well (ca. 0.9 kcal/mol) surrounding the methyl group (-CH(3)) has been found and ascribed to the interaction between an unoccupied molecular orbital of CH(3)CN and 2s atomic orbital of He*(2(3)S).