Electron diffraction self-imaging of molecular fragmentation in two-step double ionization of water.

We doubly ionize H(2)O by single photon absorption at 43 eV leading to H(+) + OH(+). A direct double ionization and a sequential process in which single ionization is followed by rapid dissociation into a proton and an autoionizing OH(*) are identified. The angular distribution of this delayed autoionization electron shows a preferred emission in the direction of the emitted proton. From this diffraction feature we obtain internuclear distances of 700 to 1100 a.u. at which the autoionization of the OH(*) occurs. The experimental findings are in line with calculations of the excited potential energy surfaces and their lifetimes.

Ionization dynamics of helium dimers in fast collisions with He++.

By employing the cold target recoil ion momentum spectroscopy technique, we have investigated the (He+, He+) breakup of a helium dimer (He2) caused by transfer ionization and double capture in collisions with alpha particles (E = 150 keV/u). Surprisingly, the results show a two-step process as well as a one-step process followed by electron exchange. In addition, interatomic Coulombic decay [L. S. Cederbaum, J. Zobeley, and F. Tarantelli, Phys. Rev. Lett. 79, 4778 (1997).] is observed in an ion collision for the first time.

Fragmentation dynamics of CO(2)(3+) investigated by multiple electron capture in collisions with slow highly charged ions.

Fragmentation of highly charged molecular ions or clusters consisting of more than two atoms can proceed in a one step synchronous manner where all bonds break simultaneously or sequentially by emitting one ion after the other. We separated these decay channels for the fragmentation of CO(2)(3+) ions by measuring the momenta of the ionic fragments. We show that the total energy deposited in the molecular ion is a control parameter which switches between three distinct fragmentation pathways: the sequential fragmentation in which the emission of an O(+) ion leaves a rotating CO(2+) ion behind that fragments after a time delay, the Coulomb explosion and an in-between fragmentation--the asynchronous dissociation. These mechanisms are directly distinguishable in Dalitz plots and Newton diagrams of the fragment momenta. The CO(2)(3+) ions are produced by multiple electron capture in collisions with 3.2 keV/u Ar(8+) ions.

Correlated electron emission in multiphoton double ionization

Electronic correlations govern the dynamics of many phenomena in nature, such as chemical reactions and solid state effects, including superconductivity. Such correlation effects can be most clearly investigated in processes involving single atoms. In particular, the emission of two electrons from an atom--induced by the impact of a single photon, a charged particle or by a short laser pulse--has become the standard process for studies of dynamical electron correlations. Atoms and molecules exposed to laser fields that are comparable in intensity to the nuclear fields have extremely high probabilities for double ionization; this has been attributed to electron-electron interaction. Here we report a strong correlation between the magnitude and the direction of the momentum of two electrons that are emitted from an argon atom, driven by a femtosecond laser pulse (at 38 TW cm(-2)). Increasing the laser intensity causes the momentum correlation between the electrons to be lost, implying that a transition in the laser-atom coupling mechanism takes place.

Complete photo-fragmentation of the deuterium molecule.

All properties of molecules--from binding and excitation energies to their geometry--are determined by the highly correlated initial-state wavefunction of the electrons and nuclei. Details of these correlations can be revealed by studying the break-up of these systems into their constituents. The fragmentation might be initiated by the absorption of a single photon, by collision with a charged particle or by exposure to a strong laser pulse: if the interaction causing the excitation is sufficiently understood, the fragmentation process can then be used as a tool to investigate the bound initial state. The interaction and resulting fragment motions therefore pose formidable challenges to quantum theory. Here we report the coincident measurement of the momenta of both nuclei and both electrons from the single-photon-induced fragmentation of the deuterium molecule. The results reveal that the correlated motion of the electrons is strongly dependent on the inter-nuclear separation in the molecular ground state at the instant of photon absorption.

Absolute ion detection efficiencies of microchannel plates and funnel microchannel plates for multi-coincidence detection.

Modern momentum imaging techniques allow for the investigation of complex molecules in the gas phase by detection of several fragment ions in coincidence. For these studies, it is of great importance that the single-particle detection efficiency ε is as high as possible, as the overall efficiency scales with εn, i.e., the power of the number of detected particles. Here we present measured absolute detection efficiencies for protons of several micro-channel plates (MCPs), including efficiency enhanced "funnel MCPs." Furthermore, the relative detection efficiency for two-, three-, four-, and five-body fragmentation of CHBrClF has been examined. The "funnel" MCPs exhibit an efficiency of approximately 90%, gaining a factor of 24 (as compared to "normal" MCPs) in the case of a five-fold ion coincidence detection.

Atomic dynamics in single and multi-photon double ionization: An experimental comparison.

We have used a multi-particle imaging technique (COLTRIMS) to observe the double ionization of rare gas atoms by multi-photon absorption of 800 nm (1.5 eV) femto-second laser pulses and by single photon absorption (synchrotron radiation). Both processes are mediated by electron correlation. We discuss similarities and differences in the three-body final state momentum distributions.

Recoil-Ion momentum distributions for single and double ionization of helium in strong laser fields

We have measured the momentum distributions of singly and doubly charged helium ions created in the focus of 220 fs, 800 nm laser pulses at intensities of (2.9-6.6)x10(14) W/cm(2). All ions are emitted strongly aligned along the direction of polarization of the light. We find the typical momenta of the He2+ ions to be 5-10 times larger than those of the He1+ ions and a two peak structure at the highest intensity.

Photo- and auger-electron recoil induced dynamics of interatomic Coulombic decay.

At photon energies near the Ne K edge it is shown that for 1s ionization the Auger electron, and for 2s ionization the fast photoelectron, launch vibrational wave packets in a Ne dimer. These wave packets then decay by emission of a slow electron via interatomic Coulombic decay (ICD). The measured and computed ICD electron spectra are shown to be significantly modified by the recoil induced nuclear motion.

Ultrafast probing of core hole localization in N2.

Although valence electrons are clearly delocalized in molecular bonding frameworks, chemists and physicists have long debated the question of whether the core vacancy created in a homonuclear diatomic molecule by absorption of a single x-ray photon is localized on one atom or delocalized over both. We have been able to clarify this question with an experiment that uses Auger electron angular emission patterns from molecular nitrogen after inner-shell ionization as an ultrafast probe of hole localization. The experiment, along with the accompanying theory, shows that observation of symmetry breaking (localization) or preservation (delocalization) depends on how the quantum entangled Bell state created by Auger decay is detected by the measurement.

Interference in the collective electron momentum in double photoionization of H2.

We investigate single-photon double ionization of H(2) by 130 to 240 eV circularly polarized photons. We find a double slitlike interference pattern in the sum momentum of both electrons in the molecular frame which survives integration over all other degrees of freedom. The difference momentum and the individual electron momentum distributions do not show such a robust interference pattern. We show that this interference results from a non-Heitler-London fraction of the H(2) ground state where both electrons are at the same atomic center.

Single photon-induced symmetry breaking of H2 dissociation.

H2, the smallest and most abundant molecule in the universe, has a perfectly symmetric ground state. What does it take to break this symmetry? We found that the inversion symmetry can be broken by absorption of a linearly polarized photon, which itself has inversion symmetry. In particular, the emission of a photoelectron with subsequent dissociation of the remaining H+2 fragment shows no symmetry with respect to the ionic H+ and neutral H atomic fragments. This lack of symmetry results from the entanglement between symmetric and antisymmetric H+2 states that is caused by autoionization. The mechanisms behind this symmetry breaking are general for all molecules.

Experimental separation of virtual photon exchange and electron transfer in interatomic coulombic decay of neon dimers.

We investigate the interatomic Coulombic decay (ICD) of neon dimers following photoionization with simultaneous excitation of the ionized atom (shakeup) in a multiparticle coincidence experiment. We find that, depending on the parity of the excited state, which determines whether ICD takes place via virtual dipole photon emission or overlap of the wave functions, the decay happens at different internuclear distances, illustrating that nuclear dynamics heavily influence the electronic decay in the neon dimer.