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Observation of accurate ion dissociation thresholds in pulsed field ionization-photoelectron studies.

We report the first observation, together with a mechanism for such an observation, of a steplike feature in the pulsed field ionization photoelectron measurement of CH4(C2H2), marking the 0 K dissociation threshold for the formation of CH3(+) + H(C2H(+) + H) from CH4(C2H2). The nonexistence of a step in the spectrum for C 2H4 at its dissociation threshold for C2H2(+) formation provides strong support for the proposed mechanism. This experiment shows that, for a range of molecules, where the ion dissociation lifetimes near the dissociation thresholds are <10(-7) s, pulsed field ionization photoelectron measurements will yield not only highly accurate ionization energies, but also 0 K dissociation thresholds.

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Photofragmentation of Na2+ in intense femtosecond laser fields: from photodissociation on light-induced potentials to field ionization.

Photofragmentation of Na2 + molecules in well prepared vibrational levels has been studied employing intense ( 10(11)-10(14) W/cm2) and ultrashort (80 fs) 790 nm laser fields. Four fragmentation channels with different released kinetic energies are observed. Depending on the applied laser intensity, the fragmentation of Na2 + is governed by photodissociation on light-induced potentials and field ionization followed by Coulomb explosion. Below 1x10(12) W/cm2, only photodissociation on light-induced potentials is seen. For intermediate laser intensities, field ionization at large internuclear distances competes with photodissociation, thus preventing the observation of above threshold dissociation. Field ionization at small internuclear distances dominates for the highest laser intensities used.

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Deep-core dielectronic-capture resonances in the electron-impact ionization of heavy atomic ions.

Experimental measurements and theoretical calculations are carried out for the electron-impact ionization of Sm(12+). The low energy region of the single ionization cross section for Sm(12+) is found to be dominated by contributions from the indirect process of excitation autoionization. At about 1.0 keV strong resonance features are found in the experimental crossed-beam measurements performed in scan mode at high resolution. Theoretical calculations confirm that the high energy experimental features are due to deep-core dielectronic capture followed by sequential double Auger decay. The discovery of these unusual high energy resonances in single and multiple ionization opens the door for future systematic studies of how heavy atomic ions with deep inner-shell vacancies achieve final stabilization.

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Microwave ionization of an atomic electron wave packet.

A short microwave pulse is used to ionize a lithium Rydberg wave packet launched from the core at a well-defined phase of the field. We observe a strong dependence on the relative phase between the motion of the wave packet and the oscillations of the field. This phase dependent ionization is also studied as a function of the relative frequency. Our experimental observations are in good qualitative agreement with a one-dimensional classical model of wave packet ionization.

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Measurement of ultrafast ionization dynamics of gases by multipulse interferometric frequency-resolved optical gating.

Ultrafast ionization dynamics of femtosecond laser-irradiated noble and simple diatomic gases were studied using a novel two-color time-domain technique which eliminated significant complications seen in past experiments. Ultrafast depletion of the probing laser pulse was observed strictly coincident with the ionization front and attributed to a previously unobserved nonlinear frequency mixing via the transverse plasma current [F. Brunel, J. Opt. Soc. Am. B 7, 52 (1990)]. Good quantitative agreement of the measured single-atom ionization rates with Ammosov-Delone-Krainov rates was found, except for O (2) which showed a 200x smaller rate.

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Suppression of multiple ionization of atomic ions in intense ultrafast laser pulses.

The interaction of an intense laser field with a beam of atomic ions has been investigated experimentally for the first time. The ionization dynamics of Ar+ ions and Ar neutrals in a 60 fs, 790 nm laser pulse have been compared and contrasted at intensities up to 10(16) W cm-2. Our results show that nonsequential ionization from an Ar+ target is strongly suppressed compared with that from the corresponding neutral target. We have also observed for the first time the strong field ionization of high lying target metastable levels in the Ar+ beam.

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Slow-down collisions and nonsequential double ionization in classical simulations.

We use classical simulations to analyze the dynamics of nonsequential double-electron short-pulse photoionization. We utilize a microcanonical ensemble of 10(5) two-electron "trajectories," a number large enough to provide large subensembles and even sub-subensembles associated with double ionization. We focus on key events in the final doubly ionized subensemble and back-analyze the subensemble's history, revealing a classical slow-down scenario for nonsequential double ionization. We analyze the dynamics of these slow-down collisions and find that a good phase match between the motions of the electrons can lead to very effective energy transfer, followed by escape over a suppressed barrier.

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Orbital picture of ionization and its breakdown in nanoarrays of quantum dots.

We present exact numerical results indicating that ionization could be a useful tool to study electron correlations in artificial molecules and nanoarrays of metallic quantum dots. For nanorings consisting of Ag quantum dots of the type already fabricated, we demonstrate that the molecular orbital picture breaks down even for lowest energy ionization processes, in contrast to ordinary molecules. Our ionization results yield a transition point between localization and delocalization regimes in good agreement with various experimental data.

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Strong field atomic ionization: origin of high-energy structures in photoelectron spectra.

Two distinct interpretations have been proposed to account for conspicuous enhancements of the ionization peaks in the high energy part of above-threshold ionization spectra. One of them ascribes the enhancement to a multiphoton resonance involving an excited state, while other analysis performed for zero-range model potential link it to "channel closings, " i.e., to the change in the number of photons needed to ionize the atom when the laser intensity increases. We report the results of model calculations that confirm the existence of a resonant process in atoms and shed light on why short-range potential models can mimic the experimental observations.

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Above threshold ionization in tightly focused, strongly relativistic laser fields.

The dynamics of electrons ionized from high charge states by lasers with intensity >10(20) W/cm(2) have been studied. At these intensities vxB forces drive the electrons subsequent to ionization in a trajectory nearly parallel to the laser propagation direction. This gives rise to large energy gains as the electron rides in phase with the laser field over a long distance. Monte Carlo simulations illustrate that, unlike in case of ionization in sub- and near-relativistic intensity fields (<10(19) W/cm(2)), the electron dynamics in the ultrarelativistic case are strongly influenced by the longitudinal electric fields found near the focus of a tightly focused laser.

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Alignment-dependent strong field ionization of molecules.

We demonstrate a method to measure strong field laser ionization of aligned molecules. The method employs a macroscopic field-free dynamic alignment, which occurs during revivals of rotational wave packets produced by a femtosecond laser pulse. We investigate the dependence of strong field ionization of N2 on molecular orientation. We determine that N2 molecules are four times more likely to ionize when aligned parallel to the field than when aligned perpendicular to it.

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Time-resolved double ionization with few cycle laser pulses.

Ionization of D2 launches a vibrational wave packet on the ground state of D+2. Removal of the second electron places a pair of D+ ions onto a Coulombic potential. Measuring the D+ kinetic energy determines the time delay between the first and the second ionization. Caught between a falling ionization and a rapidly rising intensity, the typical lifetime of the D+2 intermediate is less than 5 fs when an intense 8.6 fs laser pulse is used. We simulate Coulomb explosion imaging of the ground state wave function of D2 by a 4 fs optical pulse and compare with our experimental observations.

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Intense-laser-field ionization of molecular hydrogen in the tunneling regime and its effect on the vibrational excitation of H2+.

H2 molecules were ionized by Ti:sapphire (45 fs, 800 nm) and Nd-doped yttrium aluminum garnet lasers (6 ns, 1064 nm). The relative populations of the vibrational levels of the H+2 ions were determined and found to be concentrated in the lowest vibrational levels. Tunneling ionization calculations with exact field-modified potential curves reproduce the experimental results. The reason for the departure from conventional Franck-Condon-like distributions is the rapid variation of the ionization rate with internuclear distance.

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Influence of molecular structure on double ionization of N2 and O2 by high intensity ultrashort laser pulses.

The electron momentum correlation after nonsequential double ionization of N2 and O2 in ultrashort light pulses at light intensities near 1.5 x 10(14) W/cm(2) has been investigated. The experimental results reveal distinctive differences between the molecular species and between molecules and atoms of similar ionization threshold. We provide evidence that recollision double ionization is the essential mechanism and trace the origin of the differences back to the symmetry of the orbitals occupied by the valence electrons.

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Mutual projectile-target ionization via the two-center dielectronic interaction in relativistic ion-atom collisions.

We study mutual ionization in relativistic collisions between hydrogenlike projectiles and helium atoms: X(Z+)(1s)+He(1s(2))-->X((Z+1)+)+ He+(1s)+2e(-). At high collision velocities and for not too heavy projectiles, 2Z/v<<1 (v is the collision velocity), the mutual ionization proceeds via the direct interaction between two electrons bound (initially) to different colliding particles. Considering for the first time this fundamental process in the case of relativistic collisions, we calculate ionization cross sections and discuss manifestations of relativistic effects. In particular, we predict two novel and interesting phenomena: (i) considerable relativistic effects in collisions with low Lorentz factors gamma and (ii) the rapid saturation of these effects at higher gamma. Estimates show that the predicted effects can be experimentally tested using existing facilities and spectrometers.

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Ionization of atoms by the spatial gradient of the pondermotive potential in a focused laser beam.

Ionization of atoms by the spatial gradient of the pondermotive potential in a focused laser beam is investigated. Rydberg ions, formed during the interaction of noble gas atoms with an intense laser pulse, are used to probe the gradient field. Rydberg ion species with higher ionization potentials are produced at locations where the gradient field is largest. The measured Rydberg ion yields differ dramatically from estimates that ignore gradient-field ionization, but are in good agreement with predictions that include the effect.

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Nonsequential double ionization at the single-optical-cycle limit.

We report differential measurements of Ar++ ion momentum distributions from nonsequential double ionization in phase-stabilized few-cycle laser pulses. The distributions depend strongly on the carrier-envelope (CE) phase. Via control over the CE phase one is able to direct the nonsequential double-ionization dynamics. Data analysis through a classical model calculation reveals that the influence of the optical phase enters via (i) the cycle dependent electric field ionization rate, (ii) the electron recollision time, and (iii) the accessible phase space for inelastic collisions. Our model indicates that the combination of these effects allows a look into single cycle dynamics already for few-cycle pulses.

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