Carbon K-shell Photo Ionization of CO: Molecular frame angular Distributions of normal and conjugate shakeup Satellites

We have measured the molecular frame angular distributions of photoelectrons emitted from the Carbon K shell of fixed-in-space CO molecules for the case of simultaneous excitation of the remaining molecular ion. Normal and conjugate shake up states are observed. Photo electrons belonging to normal \Sigma -satellite lines show an angular distribution resembling that observed for the main photoline at the same electron energy. Surprisingly a similar shape is found for conjugate shake up states with \Pi -symmetry. In our data we identify shake rather than electron scattering (PEVE) as the mechanism producing the conjugate lines. The angular distributions clearly show the presence of a \Sigma -shape resonance for all of the satellite lines.Comment: 8 pages, 2 figure

Two-particle interference of electron pairs on a molecular level

We investigate the photo-doubleionization of $H_2$ molecules with 400 eV photons. We find that the emitted electrons do not show any sign of two-center interference fringes in their angular emission distributions if considered separately. In contrast, the quasi-particle consisting of both electrons (i.e. the "dielectron") does. The work highlights the fact that non-local effects are embedded everywhere in nature where many-particle processes are involved

Determination of the He-He, Ne-Ne, Ar-Ar, and H2_{2} interaction potential by wave function imaging

We report on a direct method to measure the internuclear potential energy curve of diatomic systems. A COLTRIMS reaction microscope was used to measure the squares of the vibrational wave functions of H$_{2}$, He$_{2}$, Ne$_{2}$, and Ar$_{2}$. The Schr\"odinger equation relates the curvature of the wave function to the potential V(R) and therefore offers a simple but elegant way to extract the shape of the potential.Comment: 15 pages with 4 figure

Ultrafast temporal evolution of interatomic Coulombic decay in NeKr dimers

We investigate interatomic Coulombic decay in NeKr dimers after neon inner-valence photoionization [Ne+(2s-1)] using a synchrotron light source. We measure with high energy resolution the two singly charged ions of the Coulomb-exploding dimer dication and the photoelectron in coincidence. By carefully tracing the post-collision interaction between the photoelectron and the emitted ICD electron we are able to probe the temporal evolution of the state as it decays. Although the ionizing light pulses are 80 picoseconds long, we determine the lifetime of the intermediate dimer cation state and visualize the contraction of the nuclear structure on the femtosecond time scale

Mechanisms of photo double ionization of helium by 530 eV photons

We have measured fully differential cross sections for photo double ionization of helium 450eV above the threshold. We have found an extremely asymmetric energy sharing between the photoelectrons and an angular asymmetry parameter β≃2 and β≃0 for the fast and slow electrons, respectively. The electron angular distributions show a dominance of the shakeoff for 2eV electrons and clear evidence of an inelastic electron-electron scattering at an electron energy of 30eV. The data are in excellent agreement with convergent close-coupling calculations

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

Ejection of quasi-free electron pairs from the helium atom ground state by single photon absorption

We investigate single photon double ionization (PDI) of helium at photon energies of 440 and 800 eV. We observe doubly charged ions with close to zero momentum corresponding to electrons emitted back-to-back with equal energy. These slow ions are the unique fingerprint of an elusive quasi-free PDI mechanism predicted by Amusia et al. nearly four decades years ago [J. Phys. B 8, 1248, (1975)] . It results from the non-dipole part of the electromagnetic interaction. Our experimental data are in excellent agreement with calculations performed using the convergent close coupling and time dependent close coupling methods

Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions

Citation: McCurdy, C. W., Rescigno, T. N., Trevisan, C. S., Lucchese, R. R., Gaire, B., Menssen, A., . . . Weber, T. (2017). Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions. Physical Review A, 95(1). doi:10.1103/PhysRevA.95.011401A dramatic symmetry breaking in K-shell photoionization of the CF4 molecule in which a core-hole vacancy is created in one of four equivalent fluorine atoms is displayed in the molecular frame angular distribution of the photoelectrons. Observing the photoejected electron in coincidence with an F+ atomic ion after Auger decay is shown to select the dissociation path where the core hole was localized almost exclusively on that atom. A combination of measurements and ab initio calculations of the photoelectron angular distribution in the frame of the recoiling CF3+ and F+ atoms elucidates the underlying physics that derives from the Ne-like valence structure of the F(1s-1) core-excited atom. © 2017 American Physical Society

Single photon double ionization of Helium at 800 eV - observation of the Quasi Free Mechanism

In a kinematically complete experiment we have measured the photo double ionization of Helium at aphoton energy of 800 eV and observed He2+ ions with 0 momentum, corresponding to a back-to-back-emissionof the two electrons. The results are in good agreement with theoretical calculations

Imaging the square of the correlated two-electron wave function of a hydrogen molecule

The toolbox for imaging molecules is well-equipped today. Some techniques visualize the geometrical structure, others the electron density or electron orbitals. Molecules are many-body systems for which the correlation between the constituents is decisive and the spatial and the momentum distribution of one electron depends on those of the other electrons and the nuclei. Such correlations have escaped direct observation by imaging techniques so far. Here, we implement an imaging scheme which visualizes correlations between electrons by coincident detection of the reaction fragments after high energy photofragmentation. With this technique, we examine the H2two-electron wave function in which electron-electron correlation beyond the mean-field level is prominent. We visualize the dependence of the wave function on the internuclear distance. High energy photoelectrons are shown to be a powerful tool for molecular imaging. Our study paves the way for future time resolved correlation imaging at FELs and laser based X-ray sourcesThis work was funded by the Deutsche Forschungsgemeinschaft, the BMBF, the European Research Council under the European Union Seventh Framework Programme (FP7/2007-2013)/ERC grant agreement 290853 XCHEM, the MINECO projects FIS2013-42002-R and FIS2016-77889-R, and the European COST Action XLIC CM1204. All calculations were performed at the CCC-UAM and Mare Nostrum Supercomputer Centers. We are grateful to the staff of PETRA III for excellent support during the beam time. K.M. and M.M. would like to thank the DFG for support via SFB925/A3. A.K. and V.S. thank the Wilhelm und Else Heraeus-Foundation for support. J.L. would like to thank the DFG for support. S.K. acknowledges support from the European Cluster of Advanced Laser Light Sources (EUCALL) project which has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 654220. T.W. was supported by the U.S. Department of Energy Basic Energy Sciences under Contract No. DE-AC02-05CH11231. A.P. acknowledges a Ramón y Cajal contract from the Ministerio de Economa y Competitivida