We present ultra-high-resolution COLTRIMS data on single ionization of helium induced by 1 MeV proton impact and compare it with theoretical calculations. Our analysis clearly shows the limitations of the first Born approximation.

We present ultrahigh-resolution data on fully differential cross sections for single ionization of helium induced by 1 MeV proton impact. In the present work we explore a different regime of kinematic conditions in terms of momentum transfer and electron energies than previously published data. These data are compared with different theoretical calculations. Reasonable agreement between the first Born approximation and experiment is obtained in the kinematic regime close to the Bethe ridge. Far from this region the calculated binary peak is shifted with respect to experiment. In order to resolve this problem, we analyze several theoretical mechanisms beyond the customary first Born approximation theory. These mechanisms include the 3C model (three Coulomb functions), effective charges, off-shell pair $T$ matrices instead of pair potentials, and semiclassical postcollision interaction. We find that a combination of the 3C model with a semiclassical postcollision interaction effect may explain the observed discrepancy.

The absolute configuration of individual small molecules in the gas phase can be determined directly by light-induced Coulomb explosion imaging (CEI). Herein, this approach is demonstrated for ionization with a single X-ray photon from a synchrotron light source, leading to enhanced efficiency and faster fragmentation as compared to previous experiments with a femtosecond laser. In addition, it is shown that even incomplete fragmentation pathways of individual molecules from a racemic CHBrClF sample can give access to the absolute configuration in CEI. This leads to a significant increase of the applicability of the method as compared to the previously reported complete break-up into atomic ions and can pave the way for routine stereochemical analysis of larger chiral molecules by light-induced CEI.

Molecular frame photoelectron angular distributions (MFPADs) are measured in electron-ion momentum imaging experiments and compared with complex Kohn variational calculations for carbon K-shell ionization of carbon tetrafluoride (CF4), ethane (C2H6) and 1,1-difluoroethylene (C2H2F2). While in ethane the polarization averaged MFPADs show a tendency at low energies for the photoelectron to be emitted in the directions of the bonds, the opposite effect is seen in CF4. A combination of these behaviors is seen in difluoroethylene where ionization from the two carbons can be distinguished experimentally because of their different K-shell ionization potentials. Excellent agreement is found between experiment and simple static-exchange or coupled two-channel theoretical calculations. However, simple electrostatics do not provide an adequate explanation of the suggestively simple angular distributions at low electron ejection energies.

Even though the study of ion-atom collisions is a mature field of atomic physics, large discrepancies between experiment and theoretical calculations are still common. Here we present experimental results with high momentum resolution on the single ionization of helium induced by 1-MeV protons, and we compare these to theoretical calculations. The overall agreement is strikingly good, and even the first Born approximation yields good agreement between theory and experiment. This has been expected for several decades, but so far has not been accomplished. The influence of projectile coherence effects on the measured data is briefly discussed in terms of an ongoing dispute on the existence of nodal structures in the electron angular emission distributions.

The 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.

The fully differential cross section (FDCS) for single ionization p + He → p + e + He+ at proton energy of 1 MeV is studied both experimentally and theoretically. The 3D angular electron distribution is presented. The role of electron-electron correlations both in a trial helium ground-state wave function and in the final helium state is inspected.

In this work, we show that the direct determination of a chiral molecule's absolute configuration can be achieved with Coulomb Explosion Imaging in a COLTRIMS reaction microscope. We compare the results after ionisation with femto-second laser pulses and with X-ray synchrotron light. Different fragmentation pathways of the prototypical chiral molecule CHBrClF are identified that carry information on the handedness. The applicabilty of the technique towards bigger molecules is discussed.

It's well known for atomic targets that the ionization in transfer ionization Originates from electron knock-off or initial state correlated shake-off. For H-2 molecules we have observed a similar behavior and additionally a dependency of the electron emission from the internuclear axis

We investigate orientation effects in the fragmentation of He-2 and Ne-2 induced by S14+ projectiles at an impact energy of 11.37 MeV/u. Multiple ionization shows a strong dependence on the orientation of the dimer axis with respect to the projectile beam axis. We attribute these effects to the impact-parameter-dependent ionization probability P( b) for the atomic scattering process S14+ + He and S14+ + Ne and compare our data with a Monte Carlo simulation.

We have measured the ionization and fragmentation of Helium, Neon and Argon Dimers induced by ion impact and observed two different pathways, the sequential ionization on each atom and the interatomic Coulombic decay.

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.

We report on the observation of discrete structures in the electron energy distribution for strong field double ionization of argon at 394 nm. The experimental conditions were chosen in order to ensure a nonsequential ejection of both electrons with an intermediate rescattering step. We have found discrete above-threshold ionization like peaks in the sum energy of both electrons, as predicted by all quantum mechanical calculations. More surprisingly, however, is the observation of two above-threshold ionization combs in the energy distribution of the individual electrons.

We investigate the contribution of Interatomic Coulombic Decay induced by ion impact in neon and argon dimers (Ne_2 and Ar_2) to the production of low energy electrons. Our experiments cover a broad range of perturbation strengths and reaction channels. We use 11.37 MeV/u S^14+, 0.125 MeV/u He^1+, 0.1625 MeV/u He^1+ and 0.150 MeV/u He^2+ as projectiles and study ionization, single and double electron transfer to the projectile as well as projectile electron loss processes. The application of a COLTRIMS reaction microscope enables us to retrieve the three-dimensional momentum vectors of the ion pairs of the fragmenting dimer into Ne^q+/Ne^1+ and Ar^q+/Ar^1+ (q = 1, 2, 3) in coincidence with at least one emitted electron.