Dissociative Autoionization in (1+2)-photon Above Threshold Excitation of H2 Molecules

We have theoretically studied the effect of dissociative autoionization on the photoelectron energy spectrum in (1+2)-photon above threshold ionization(ATI) of H2 molecules. We have considered excitation from the ground state X-singlet-Sigma-g+(v=0,j) to the doubly excited autoionizing states of singlet-Sigma-u+ and singlet-Pi-u+ symmetry, via the intermediate resonant B-singlet-Sigma-u+(v=5,j) states. We have shown that the photoelectron energy spectrum is oscillatory in nature and shows three distinct peaks above the photoelectron energy 0.7 eV. This feature has been observed in a recent experiment by Rottke et al, J. Phys. B, Vol. 30, p-4049 (1997).Comment: 11 pages and 4 figure

Ultrafast dynamics of neutral superexcited Oxygen: A direct measurement of the competition between autoionization and predissociation

Using ultrafast extreme ultraviolet pulses, we performed a direct measurement of the relaxation dynamics of neutral superexcited states corresponding to the nl\sigma_g(c^4\Sigma_u^-) Rydberg series of O_2. An XUV attosecond pulse train was used to create a temporally localized Rydberg wavepacket and the ensuing electronic and nuclear dynamics were probed using a time-delayed femtosecond near-infrared pulse. We investigated the competing predissociation and autoionization mechanisms for superexcited molecules and found that autoionization is dominant for the low n Rydberg states. We measured an autoionization lifetime of 92+/-6 fs and 180+/-10 fs for (5s,4d)\sigma_g and (6s,5d)\sigma_g Rydberg state groups respectively. We determine that the disputed neutral dissociation lifetime for the \nu=0 vibrational level of the Rydberg series is 1100+/-100fs.Comment: 5 pages, 4 figure

Energy dependence of the differential photoelectron cross sections of molecular nitrogen

The angular distribution of photoelectron intensity for molecular nitrogen was studied using He I and Ne I resonance line discharge light sources. Studies of photoelectron angular distributions covering a range of photon energies, and thus a range of photoelectron energies, are possible using the weaker high order lines in each discharge as well as the principal lines. Peaks in three photoelectron bands of N_2 were studied at the photon energies 16.85, 19.78, 21.22, 23.09, and 23.74 eV, where possible. We find that the v′=0 peak of the X^ 2Σ^+_g band has abnormally high intensity and, at the higher photon energies, an abnormally low angular distribution asymmetry parameter, β. Several mechanisms for this anomaly are discussed, including autoionization, the variation of electric dipole transition moments with internuclear distance, and possible shape resonance phenomena. None of these explanations is completely in agreement with all theoretical and experimental evidence

Renner-Teller effects in HCO+ dissociative recombination

A theoretical description of the dissociative recombination process for the HCO+ ion suggests that the nonadiabatic Renner-Teller coupling between electronic and vibrational degrees of freedom plays an important role. This finding is consistent with a recent study of this process for another closed-shell molecule, the H3+ ion, where Jahn-Teller coupling was shown to generate a relatively high rate. The cross section obtained here for the dissociative recombination of HCO+exhibits encouraging agreement with a merged-beam experiment.Comment: 11 page

Laser-induced fluorescence studies of HfF+ produced by autoionization

Autoionization of Rydberg states of HfF, prepared using the optical-optical double resonance (OODR) technique, holds promise to create HfF+ in a particular Zeeman level of a rovibronic state for an electron electric dipole moment (eEDM) search. We characterize a vibronic band of Rydberg HfF at 54 cm-1 above the lowest ionization threshold and directly probe the state of the ions formed from this vibronic band by performing laser-induced fluorescence (LIF) on the ions. The Rydberg HfF molecules show a propensity to decay into only a few ion rotational states of a given parity and are found to preserve their orientation qualitatively upon autoionization. We show empirically that we can create 30% of the total ion yield in a particular |J+,M+> state and present a simplified model describing autoionization from a given Rydberg state that assumes no angular dynamics.Comment: 8 pages, 5 figure

Attosecond time delay in the photoionization of Mn in the region of the 3p→3d3p \rightarrow 3d giant resonance

The initial insight into time delay in Mn photoionization in the region of the $3p \to 3d$ giant autoionization resonance is gained in the framework of the "spin-polarized" random phase approximation with exchange. The dramatic effect of the giant autoionization resonance on time delay of photoemission from the $3d$ and $4s$ valence subshells of the Mn atom is unraveled. Strong sensitivity of the time delay of the $4s$ photoemission to the final-state term of the ion-remainder [${\rm Mn^{+}}(4s^{1},$$^{5}S)$ vs.~${\rm Mn^{+}}(4s^{1},$$^{7}S)$] is discovered. It is shown that photoionization time delay in the autoionizing resonance region is explicitly associated with the resonance lifetime, which can, thus, be directly measured in attosecond time delay experiments. Similar features are expected to emerge in photoionization time delays of other transition-metal and rare-earth atoms with half-filed subshells that possess giant autoionization resonances as well.Comment: 8 pages, 4 figures, 49 reference

Contribution of high-nl shells to electron-impact ionization processes

The contribution to electron-impact ionization cross sections from excitations to high-nl shells and a consequent autoionization is investigated. We perform relativistic subconfiguration-average and detailed level-to-level calculations for this process. Ionization cross sections for the W27+ ion are presented to illustrate the large influence of the high shells (n >= 9) and orbitals (l >= 4) in the excitation-autoionization process. The obtained results show that the excitations to the high shells (n >= 9) increase cross sections of the indirect ionization process by a factor of 2 compared to the excitations to the lower shells (n <= 8). The excitations to the shells with orbital quantum number l = 4 give the largest contribution comparedwith the other orbital quantum numbers l. Radiative damping reduces the cross sections of the indirect process approximately twofold in the case of the level-to-level calculations. Determined data show that the excitation-autoionization process contributes approximately 40% to the total ionization cross sections.Comment: 18 pages including 6 figures and 2 table