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.

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.

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.

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.

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.

The simplest double slit: interference and entanglement in double photoionization of H2.

The wave nature of particles is rarely observed, in part because of their very short de Broglie wavelengths in most situations. However, even with wavelengths close to the size of their surroundings, the particles couple to their environment (for example, by gravity, Coulomb interaction, or thermal radiation). These couplings shift the wave phases, often in an uncontrolled way, and the resulting decoherence, or loss of phase integrity, is thought to be a main cause of the transition from quantum to classical behavior. How much interaction is needed to induce this transition? Here we show that a photoelectron and two protons form a minimum particle/slit system and that a single additional electron constitutes a minimum environment. Interference fringes observed in the angular distribution of a single electron are lost through its Coulomb interaction with a second electron, though the correlated momenta of the entangled electron pair continue to exhibit quantum interference.

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.

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.

Partial photoionization cross sections and angular distributions for double excitation of helium up to the N = 13 threshold.

Partial photoionization cross sections sigmaN(Egamma) and photoelectron angular distributions betaN(Egamma) were measured for the final ionic states He+ (N > 4) in the region between the N = 8 and N = 13 thresholds (Egamma > 78.155 eV) using the cold target recoil ion momentum spectroscopy technique (COLTRIMS). Comparison of the experimental data with two independent sets of theoretical predictions reveals disagreement for the branching ratios to the various HeN(+) states. The angular distributions just below the double ionization threshold suggest an excitation process for highly excited N states similar to the Wannier mechanism for double ionization.

Experimental observation of interatomic coulombic decay in neon dimers.

Recently Cederbaum et al. [Phys. Rev. Lett. 79, 4778 (1997)]] predicted a new decay channel of excited atoms and molecules termed interatomic Coulombic decay (ICD). In ICD the deexcitation energy is transferred via virtual photon exchange to a neighboring atom, which releases it by electron emission. We report on an experimental observation of ICD in 2s ionized neon dimers. The process is unambiguously identified by detecting the energy of two Ne1+ fragments and the ICD electron in coincidence, yielding a clean, background free experimental spectral distribution of the ICD electrons.

Vibrationally resolved K-shell photoionization of CO with circularly polarized light.

Diffraction of a low energy (<4 eV) carbon-K-photoelectron wave that is created inside a CO molecule by absorption of a circularly polarized photon is investigated. The measurements resolve the vibrational states of the K-shell ionized CO+ molecule and display the photoelectron diffraction patterns in the molecular frame. These show significant variation for the different vibrational states. This effect is stronger than predicted by state-of-the-art theory. As this study is performed close to C-K-threshold and, therefore, far below the molecule's sigma-shape resonance, this surprisingly strong effect is not related to that resonance phenomenon.

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.

Fully differential rates for femtosecond multiphoton double ionization of neon.

We have investigated the full three-dimensional momentum correlation between the electrons emitted from strong field double ionization of neon when the recollision energy of the first electron is on the order of the ionization potential. The momentum correlation in the direction perpendicular to the laser field depends on the time difference of the two electrons leaving the ion. Our results are consistent with double ionization proceeding through transient double excited states that field ionize.

Fully differential cross sections for photo-double-ionization of D2.

We report the first kinematically complete study of the four-body fragmentation of the D2 molecule following absorption of a single photon. For equal energy sharing of the two electrons and a photon energy of 75.5 eV, we observed the relaxation of one of the selection rules valid for He photo-double-ionization and a strong dependence of the electron angular distribution on the orientation of the molecular axis. This effect is reproduced by a model in which a pair of photoionization amplitudes is introduced for the light polarization parallel and perpendicular to the molecular axis.

Photoelectron-photoion momentum spectroscopy as a clock for chemical rearrangements: isomerization of the di-cation of acetylene to the vinylidene configuration.

We have used complete correlated momentum mapping of the photoelectron and heavy ion products from the dissociation of the di-cation of acetylene, induced by photoionizing the carbon K shell of one of the atoms, to map out the angular correlation between the electron and the axis of the target molecule. The (quasi-) symmetric decay is found to proceed through both acetylene and vinylidene configurations. By using the strongly peaked photoelectron emission to "start a clock," an upper limit of 60 fs is placed on the isomerization time from the acetylene to the vinylidene configuration.

Auger electron emission from fixed-in-space CO.

We have measured the angular distribution of carbon K-Auger electrons from fixed in space, core-ionized, CO molecules in coincidence with the kinetic energy release of the C+ and O+ fragments. We find a very narrow ejection of Auger electrons in the direction of the oxygen and an oscillatory diffraction pattern. Even for similar electron energies, the angular distribution strongly depends on the symmetry of the final state.

Mechanisms of photo double ionization of helium by 530 eV photons.

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

Direct probe of the bent and linear geometries of the core-excited Renner-Teller pair states by means of the triple-ion-coincidence momentum imaging technique.

The doubly degenerate core-excited Pi state of CO2 splits into two due to static Renner-Teller effect. Using the triple-ion-coincidence momentum imaging technique and focusing on the dependence of the measured quantities on the polarization of the incident light, we have probed, directly and separately, the linear and bent geometries for the B1 and A1 Renner-Teller pair states, as a direct proof of the static Renner-Teller effect.