Auger decay and subsequent fragmentation pathways of ethylene following K-shell ionization

Citation: Gaire, B., Haxton, D. J., Sturm, F. P., Williams, J., Gatton, A., Bocharova, I., . . . Weber, T. (2015). Auger decay and subsequent fragmentation pathways of ethylene following K-shell ionization. Physical Review A, 92(1), 13. doi:10.1103/PhysRevA.92.013408The fragmentation pathways and dynamics of ethylene molecules after core ionization are explored using coincident measurements of the Auger electron and fragment ions by employing the cold target recoil-ion momentum spectroscopy method. The influence of several factors on the dynamics and kinematics of the dissociation is studied. These include propensity rules, ionization mechanisms, symmetry of the orbitals from which the Auger electrons originate, multiple scattering, conical intersections, interference, and possible core-hole localization for the double ionization of this polyatomic molecule. Energy correlation maps allow probing the multidimensional potential energy surfaces and, in combination with our multiconfiguration self-consistent field calculations, identifying the populated electronic states of the dissociating dication. The measured angular distributions of the Auger electrons in the molecular frame further support and augment these assignments. The deprotonation and molecular hydrogen ion elimination channels show a nearly isotropic Auger electron angular distribution with a small elongation along the direction perpendicular to the molecular axis. For the symmetric breakup the angular distributions show a clear influence of multiple scattering on the outgoing electrons. The lowest kinetic energy release feature of the symmetric breakup channel displays a fingerprint of entangled Auger and photoelectron motion in the angular emission pattern identifying this transition as an excellent candidate to probe core-hole localization at a conical intersection of a polyatomic molecule.Additional Authors: Landers, A. L.;Belkacem, A.;Dorner, R.;Weber, T

INTERLAYER COUPLING AND THE METAL-INSULATOR TRANSITION IN Pr-SUBSTITUTED Bi(2)Sr(2)CaCu(2)O(8+y)

Substitution of rare-earth ions for Ca in Bi2Sr2CaCu2O8+y is known to cause a metal-insulator transition. Using resonant photoemission we study how this chemical substitution affects the electronic structure of the material. For the partial Cu-density of states at E_F and in the region of the valence band we observe no significant difference between a pure superconducting sample and an insulating sample with 60% Pr for Ca. This suggests that the states responsible for superconductivity are predomi- nately O-states. The partial Pr-4f density of states was extracted utilizing the Super- Koster-Kronig Pr 4d-4f resonance. It consists of a single peak at 1.36eV binding energy. The peak shows a strongly assymetric Doniach-Sunjic line- shape indicating the presence of a continuum of electronic states with sharp cut off at E_F even in this insulating sample. This finding excludes a bandgap in the insulating sample and supports the existance of a mobility gap caused by spatial localization of the carriers. The presence of such carriers at the Pr-site, between the CuO_2 planes shows that the electronic structure is not purely 2-dimensional but that there is a finite interlayer coupling. The resonance enhancement of the photoemission cross section, at the Pr-4d threshold, was studied for the Pr-4f and for Cu-states. Both the Pr-4f and the Cu-states show a Fano-like resonance. This resonance of Cu-states with Pr-states is another indication of coupling between the the Pr-states and those in the CuO_2 plane. Because of the statistical distribution of the Pr-ions this coupling leads to a non-periodic potential for the states in the CuO_2 plane which can lead to localization and thus to the observed metal-insulator transition.Comment: Gziped uuencoded postscript file including 7 figures Scheduled for publication in Physical Review B, May 1, 1995

Hydrogen and fluorine migration in photo-double-ionization of 1,1-difluoroethylene (1,1-C2H2F2) near and above threshold

We have studied the nondissociative and dissociative photo-double-ionization of 1,1-difluoroethylene using single photons of energies ranging from 40 to 70 eV. Applying a coincident electron-ion three-dimensional momentum imaging technique, kinematically complete measurements have been achieved. We present the branching ratios of the six reaction channels identified in the experiment. Electron-ion energy maps and relative electron emission angles are used to distinguish between direct and indirect photo-double-ionization mechanisms at a few different photon energies. The influence of selection and propensity rules is discussed. Threshold energies of double ionization are extracted from the sum of the kinetic energies of the electrons, which hint to the involvement of different manifolds of states. The dissociative ionization channels with two ionic fragments are explored in detail by measuring the kinetic energy release of the fragment ions, sum of the kinetic energies, as well as the energy sharing of the two emitted electrons. We investigate the migration of hydrogen and fluorine atoms and compare the experimental results to the photo-double-ionization of centrosymmetric linear and planar hydrocarbons (C[subscript 2]H[subscript 2] and C[subscript 2]H[subscript 4]) whenever possible

A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment

In this work we present a comprehensive and detailed study of Interatomic Coulombic Decay (ICD) occurring after irradiating argon dimers with XUV-synchrotron radiation. A manifold of different decay channels is observed and the corresponding initial and final states are assigned. Additionally, the effect of nuclear dynamics on the ICD electron spectrum is examined for one specific decay channel. The internuclear distance-dependent width Γ(R) of the decay is obtained from the measured kinetic energy release distribution of the ions employing a classical nuclear dynamics model

Mobiltelefone und Organizer als Zugangsmedien zu Informationssystemen

Die Teilnahme an Gemeinschaften in Neuen Medien setzt Zugangsgeräte voraus. Die Nutzung leistungsfähiger Universalrechner ist eine verbreitete Möglichkeit, die allerdings eine umfangreiche und kostenintensive technische Ausstattung verlangt. Deswegen ist es notwendig, ergänzend nach Wegen für einen unbeschwerten und kostensparenden Zugang zu suchen. In diesem Beitrag wird über Software-Engineering-Projekte an der FH Hamburg berichtet. In diesen Projekten wurden Informationssysteme auf einem Server entwickelt und zur Nutzung durch ein Mobiltelefon oder einen Organizer zugänglich gemacht. Hierzu wurden experimentelle und explorative Prototypen entwickelt. Damit entsteht die Möglichkeit, das Informationsangebot von gemeinschaftsbildenden Systemen mit allgegenwärtigen Geräten zu nutzen. Mit diesen Projekten wird ein Beleg dafür erbracht, dass der Ansatz und die hierzu entwickelte technische Konzeption praktikabel sind. Allerdings wird eine aus Sicht der hier diskutierten Anwendungen erforderliche Leistungssteigerung sowohl der Geräte als auch der benutzten Übertragungsdienste dringend erwartet

Photo-double-ionization of ethylene and acetylene near threshold

We present kinematically complete measurements of the photo-double-ionization of ethylene (double CC bond) and acetylene (triple CC bond) hydrocarbons just above the double-ionization threshold. We discuss the results in terms of the coincident kinetic energy of the photoelectrons and the nuclear kinetic-energy release of the recoiling ions. We have incorporated quantum chemistry calculations to interpret which of the electronic states of the dication have been populated and trace the various subsequent fragmentation channels. We suggest pathways that involve the electronic ground and excited states of the precursor ethylene dication and explore the strong influence of the conical intersections between the different electronic states. The nondissociative ionization yield is small in ethylene and high in acetylene when compared with the dissociative ionization channels. The reason for such a striking difference is explained in part on the basis of a propensity rule that influences the population of states in the photo-double-ionization of a centrosymmetric closed-shell molecule by favoring singlet ungerade and triplet gerade final states. This propensity rule and the calculated potential-energy surfaces clarify a picture of the dynamics leading to the observed dication dissociation products

A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment

In this work we present a comprehensive and detailed study of Interatomic Coulombic Decay (ICD) occurring after irradiating argon dimers with XUV-synchrotron radiation. A manifold of different decay channels is observed and the corresponding initial and final states are assigned. Additionally, the effect of nuclear dynamics on the ICD electron spectrum is examined for one specific decay channel. The internuclear distance-dependent width Γ(R) of the decay is obtained from the measured kinetic energy release distribution of the ions employing a classical nuclear dynamics model

A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment

In this work we present a comprehensive and detailed study of Interatomic Coulombic Decay (ICD) occurring after irradiating argon dimers with XUV-synchrotron radiation. A manifold of different decay channels is observed and the corresponding initial and final states are assigned. Additionally, the effect of nuclear dynamics on the ICD electron spectrum is examined for one specific decay channel. The internuclear distance-dependent width Γ(R) of the decay is obtained from the measured kinetic energy release distribution of the ions employing a classical nuclear dynamics model