Thorsten Weber

Fragmentation pathways for selected electronic states of the acetylene dication

Coincident measurement of the Auger electron and fragment ion momenta emitted after carbon core-level photoionization of acetylene has yielded new understanding of how the dication fragments. Ab initio calculations and experimental data, including body-frame Auger angular distributions, are used to identify the parent electronic states and together yield a comprehensive map of the dissociation pathways which include surface crossings and barriers to direct dissociation. The Auger angular distributions for certain breakup channels show evidence of core–hole localization. (Some figures in this article are in colour only in the electronic version)

Kinematically complete experiments using cold target recoil ion momentum spectroscopy

Abstract Cold Target Recoil Ion Momentum Spectroscopy allows the detection of the three-dimensional momentum vector of the recoiling product ion from ion, electron or photon atom collisions with 4π solid angle and high resolution. It can be combined with large area position-sensitive detectors for electron detection or measurement of the projectile charge-state and scattering angle. Such ‘reaction microscopes’ cover the full correlated momentum space of all fragments of an atomic reaction yielding kinematically complete information for each reaction event. For the first time in atomic collision physics fully differential data became available in the sense that not only the momenta of all fragments, but also the complete momentum space is observed in one experiment. Recent results achieved with this new technique for slow p-He collisions and threshold photo ionization of He will be discussed.

Evidence of interatomic Coulombic decay in ArKr after Ar 2p Auger decay

We have identified interatomic Coulombic decay (ICD) processes in the ArKr dimer following Ar 2p Auger decay, using momentum-resolved electron–ion–ion coincidence spectroscopy and simultaneously determining the kinetic energy of the ICD electron and the KER between Ar 2+ and Kr + . We find that the spin-conserved ICD processes in which Ar 2+ (3p −3 3d) 1 Pa nd 3 P decay to Ar 2+ (3p −2 ) 1 Da nd 3 P, respectively, ionizing the Kr atom, are significantly stronger than the spin-flip ICD processes in which Ar 2+ (3p −3 3d) 1 Pa nd 3 P decay to Ar 2+ (3p −2 ) 3 Pa nd 1 D, respectively. (Some figures in this article are in colour only in the electronic version)

Dynamics of the Dissociating Uracil Anion Following Resonant Electron Attachment

We report a combined experimental and theoretical investigation of dissociative electron attachment (DEA) to the nucleobase uracil. Using ion momentum imaging experiments employing a DEA reaction microscope we have measured 3-dimensional momentum distributions of specific anionic fragments following DEA to uracil by 6 eV electrons. From the measured anion fragment kinetic energy we determine the possible dissociation pathways and the total kinetic energy release. We employ electronic structure and electron scattering calculations to determine the probability for electron attachment in the molecular frame. Combining these calculations with the imaging measurements, we reveal several key features of the coupled electronic and nuclear dynamics of DEA.

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 H2 two-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 sources.Electron-electron correlation is a complex and interesting phenomenon that occurs in multi-electron systems. Here, the authors demonstrate the imaging of the correlated two-electron wave function in hydrogen molecule using the coincident detection of the electron and proton after the photoionization.

Differential cross sections in antiproton and proton-helium collisions

Cross sections are presented for the first time for antiproton-helium collisions at an energy of 945 keV differential in longitudinal electron and recoil-ion momenta. The longitudinal momentum distributions for antiproton impact are compared with 1 MeV proton-helium collision. The electron and the recoil-ion momentum distributions for antiprotons agree with those for protons to within 10%. We did not observe a difference between antiproton impact and proton impact. A comparison with CDW and CTMC theories is presented.

Time-resolved x-ray photoelectron spectroscopy techniques for real-time studies of interfacial charge transfer dynamics

X-ray based spectroscopy techniques are particularly well suited to gain access to local oxidation states and electronic dynamics in complex systems with atomic pinpoint accuracy. Traditionally, these techniques are applied in a quasi-static fashion that usually highlights the steady-state properties of a system rather than the fast dynamics that often define the system function on a molecular level. Novel x-ray spectroscopy techniques enabled by free electron lasers (FELs) and synchrotron based pump-probe schemes provide the opportunity to monitor intramolecular and interfacial charge transfer processes in real-time and with element and chemical specificity. Two complementary time-domain xray photoelectron spectroscopy techniques are presented that are applied at the Linac Coherent Light Source (LCLS) and the Advanced Light Source (ALS) to study charge transfer processes in N3 dye-sensitized ZnO semiconductor nanocrystals, which are at the heart of emerging light-harvesting technologies.

Recoil ion momentum spectroscopy a ‘momentum microscope’ to view atomic collision dynamics

Recoil ion momentum spectroscopy is a powerful tool for investigating the dynamics of ion, electron or photon impact reactions with atoms or molecules. It allows to measure the three dimensional momentum vector of the ion from those reactions with high resolution and 4 π solid angle. It can be easily combined with novel 4 π electron momentum analysers and for coincident detection of the projectile. This technique gives a complete image of the square of the correlated many body final state wave function in momentum space (i.e. fully differential cross sections) for the various reactions. The application to photo double ionization of helium by linear and circular polarized light is discussed.

Electron Localization in Dissociating H2+ by Retroaction of a Photoelectron onto Its Source

We investigate the dissociation of H_{2}^{+} into a proton and a H^{0} after single ionization with photons of an energy close to the threshold. We find that the p^{+} and the H^{0} do not emerge symmetrically in the case of the H_{2}^{+} dissociating along the 1sσ_{g} ground state. Instead, a preference for the ejection of the p^{+} in the direction of the escaping photoelectron can be observed. This symmetry breaking is strongest for very small electron energies. Our experiment is consistent with a recent prediction by Serov and Kheifets [Phys. Rev. A 89, 031402 (2014)]. In their model, which treats the photoelectron classically, the symmetry breaking is induced by the retroaction of the long-range Coulomb potential onto the dissociating H_{2}^{+}.

From Atoms to Molecules

In the present chapter, we discuss direct photo double ionization by singlephoton absorption (Sect. 14.2) and Compton scattering (Sect. 14.3). We do not discuss the closely related phenomenon of multiple ionization by two-step processes such as photoionization followed by single- or multiple-Auger decay. We concentrate on the two most fundamental two-electron target systems: the helium atom (Sects. 14.2 and 14.3) and molecular hydrogen (deuterium) (Sect. 14.4). The subject of photo double ionization of helium is now a mature field in which an impressive experimental and theoretical breakthrough has been achieved in the previous 10 years. The theoretical progress is described in Part III of this book, we therefore restrict ourselves here to a phenomenological description and intuitive interpretation of the physical phenomena. For the problem of two-electron processes in molecules, in contrast, the major challenges for experimentalist and theoretician still lie ahead.