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

Strongly Enhanced Backward Emission of Electrons in Transfer and Ionization

We studied three-dimensional angular distributions and longitudinal momentum spectra of electrons ejected in transfer plus ionization (TI), i.e., the ejection of one and the capture of a second target electron, for ion-helium collisions. We observe a pronounced structure strongly focused opposite to the projectile beam direction, which we associate with a new correlated TI mechanism proposed recently. This process contributes significantly to the total cross sections over a broad range of perturbations η, even at η as large as 0.5, where uncorrelated TI mechanisms were thought to be dominant

Interatomic Coulombic decay following the Auger decay: Experimental evidence in rare-gas dimers

Interatomic Coulombic decay (ICD) in Ar(2), ArKr and Kr(2) following Ar 2p or Kr 3d Auger decay has been investigated by means of momentum-resolved electron-ion-ion coincidence spectroscopy. This sequential decay leads to Coulombic dissociation into dication and monocation. Simultaneously determining the kinetic energy of the ICD electron and the kinetic energy release between the two atomic ions, we have been able to unambiguously identify the ICD channels. We find that, in general, spin-conserved ICD, in which the singlet (triplet) dicationic state produced via the atomic Auger decay preferentially decays to the singlet (triplet) state, transferring the energy to the other atom, is faster than spin-flip ICD, in which the Auger final singlet (triplet) dicationic state decays to the triplet (singlet) state. However, spin-flip ICD may take place when spin-conserved ICD becomes energetically forbidden. Dipole-forbidden ICDs from Kr(2+)(4s(-2) (1)S)-B (B = Ar or Kr) to Kr(2+)(4p(-2) (1)D, (3)P)-B(+) are also observed. (c) 2008 Elsevier B.V. All rights reserved

Fragmentation pathwaysfor selected electronic states of theacetylene dication

Coincident measurement of the Auger electron and fragmention momenta emitted after carbon core-level photoionization of acetylenehas yielded new understanding of how the dication fragments. Ab initiocalculations and experimental data, including body-frame Auger angulardistributions, are used to identify the parent electronic states andtogether yield a comprehensive map of the dissociation pathways whichinclude surface crossings and barriers to direct dissociation. The Augerangular distributions show evidence of core-holelocalization

Roadmap on photonic, electronic and atomic collision physics: I. Light-matter interaction

We publish three Roadmaps on photonic, electronic and atomic collision physics in order to celebrate the 60th anniversary of the ICPEAC conference. In Roadmap I, we focus on the light-matter interaction. In this area, studies of ultrafast electronic and molecular dynamics have been rapidly growing, with the advent of new light sources such as attosecond lasers and x-ray free electron lasers. In parallel, experiments with established synchrotron radiation sources and femtosecond lasers using cutting-edge detection schemes are revealing new scientific insights that have never been exploited. Relevant theories are also being rapidly developed. Target samples for photon-impact experiments are expanding from atoms and small molecules to complex systems such as biomolecules, fullerene, clusters and solids. This Roadmap aims to look back along the road, explaining the development of these fields, and look forward, collecting contributions from twenty leading groups from the field

Angular Scattering in Fast Ion-Atom Electron Transfer Collisions: Projectile Wave Diffraction and Thomas Mechanisms

We report experimental angular differential cross sections for double-electron capture in He2+ + He collisions and single-electron capture in H+ + He collisions for the 1.3-12.5 MeV kinetic energy range. In all cases, the total cross sections are dominated by forward scattering peaks in dσ/dΩ. The shapes and widths (but not the magnitudes) of these peaks are very similar for all energies and for capture of one or two electrons corresponding also to our measured linear increases in the transverse momentum transfers with increasing projectile velocities. These observations may be ascribed to diffraction limitations which are connected to electron transfer probabilities P(b) which are significant in limited regions of b only. For the H+ + He single-electron capture we observe two additional maxima in the angular differential cross sections. We conclude that while the secondary maxima at ~0.5 mrad probably have large contributions from the Thomas proton-electron-nucleus scattering mechanism, the third maxima at ~0.75 mrad are most likely mainly due to projectile de Broglie wave diffraction

Two-Center Double-Capture Interference in Fast H e²⁺+ H₂ Collisions

We report the first observation of Young-type interference effects in a two-electron transfer process. These effects change strongly as the projectile velocity changes in fast (1.2 and 2.0 MeV) He2++H2 collisions as manifested in strong variations of the double-electron capture rates with the H2 orientation. This is consistent with fully quantum mechanical calculations, which ignore sequential electron transfer, and a simple projectile de Broglie wave picture assuming that two-electron transfer probabilities are higher in collisions where the projectile passes close to either one of the H2 nuclei