Attosecond Strobing of Two-Surface Population Dynamics in DissociatingH2+ (original) (raw)

Two-photon double ionization of H_{2} in intense femtosecond laser pulses

Physical Review A, 2010

Triple-differential cross sections for two-photon double ionization of molecular hydrogen are presented for a central photon energy of 30 eV. The calculations are based on a fully ab initio, nonperturbative, approach to the time-dependent Schrödinger equation in prolate spheroidal coordinates, discretized by a finite-element discrete-variable-representation. The wave function is propagated in time for a few femtoseconds using the short, iterative Lanczos method to study the correlated response of the two photoelectrons to short, intense laser radiation. The current results often lie in between those of Colgan et al [J. Phys. B 41 (2008) 121002] and Morales et al [J. Phys. B 41 (2009) 134013]. However, we argue that these individual predictions should not be compared directly to each other, but preferably to experimental data generated under well-defined conditions. PACS numbers: 33.80.-b, 33.80.Wz, 31.15.A-

Attosecond electro-nuclear dynamics of H2 double ionization

2007

The ultrafast electronic and nuclear dynamics of H2 laser-induced double ionization is studied using a time-dependent wave packet approach that goes beyond the fixed nuclei approximation. The different double ionization pathways are analyzed by following the evolution of the total wave function during and after the pulse. We show that the rescattering of the first ionized electron produces a coherent superposition of excited molecular states which presents a pronounced transient ionic character. This attosecond excitation is followed by field-induced double ionization and by the formation of short-lived autoionizing states which decay via double ionization. These two different double ionization mechanisms may be identified by their signature imprinted in the kinetic-energy distribution of the ejected protons.

Ionization and dissociation dynamic of H 2 molecule driven by a laser field

We study the single and double ionization yields and the dissociation dynamics of a one-dimensional two-electron molecule exposed to an intense laser pulse. The double ionization yields are systematically investigated for both fixed and moveable nuclei. At low intensities the ionization curves have a power law shape, followed by a knee profile for higher intensities. A temporal correlation between the nuclear motion and the electron ionization shows that the nuclear motion deeply affects the ionization yield.

Ultrafast Electronuclear Dynamics of H2 Double Ionization

Physical Review Letters, 2007

The ultrafast electronic and nuclear dynamics of H2 laser-induced double ionization is studied using a time-dependent wave packet approach that goes beyond the fixed nuclei approximation. The double ionization pathways are analyzed by following the evolution of the total wave function during and after the pulse. The rescattering of the first ionized electron produces a coherent superposition of excited molecular states which presents a pronounced transient H + H − character. This attosecond excitation is followed by field-induced double ionization and by the formation of short-lived autoionizing states which decay via double ionization. These two double ionization mechanisms may be identified by their signature imprinted in the kinetic-energy distribution of the ejected protons.

The dynamical behaviour of H2 and D2 in a strong, femtosecond laser field

Detailed measurements of H 2 and D 2 dissociation fragment kinetic energy dependences on laser intensity, using 150 fs, 800 nm pulses, are presented. The yields for both molecular and atomic ions are also given. The observed three-peak kinetic energy spectrum carries within it the signature of the different stages of the interaction. The two lower energy peaks are a product of bond softening (and above threshold) dissociation of the molecular ion from Franck-Condon populated vibrational levels. The third higher-energy peak results from enhanced ionization of the dissociating molecular ions. No light-induced vibrational trapping need be invoked to interpret the higher-energy fragments.

Enhanced ionization of theH2molecule driven by intense ultrashort laser pulses

Physical Review A, 2010

We report correlated two-electron ab initio calculations for the hydrogen molecule H 2 in interaction with intense ultrashort laser pulses, via a solution of the full three-dimensional time-dependent Schrödinger equation. Our results for ionization and excitation probabilities (at 800 and 400 nm) as a function of internuclear distance R show strong evidence of enhanced ionization, in both single and double ionization, as well as enhanced excitation, in single and double excitation, as the internuclear distance R increases from the equilibrium value R e. The enhancement of all these molecular processes exhibits a maximum at a critical distance R c , which can be predicted from simple electrostatic and recollision models.

Attosecond control in photoionization of hydrogen molecules

2011

We report experiments where hydrogen molecules were dissociatively ionized by an attosecond pulse train in the presence of a near-infrared field. Fragment ion yields from distinguishable ionization channels oscillate with a period that is half the optical cycle of the IR field. For molecules aligned parallel to the laser polarization axis, the oscillations are reproduced in two-electron quantum simulations, and can be explained in terms of an interference between ionization pathways that involve different harmonic orders and a laser-induced coupling between the 1s g and 2p u states of the molecular ion. This leads to a situation where the ionization probability is sensitive to the instantaneous polarization of the molecule by the IR electric field and demonstrates that we have probed the IR-induced electron dynamics with attosecond pulses.

Two-color coherent control of H+2 photodissociation in intense laser fields

Physical Review Letters, 1993

We study the multiphoton dissociation of H2 + by a coherent superposition of an intense short pulsed laser radiation and one of its harmonies (second or third), in a phase-Iocked regime. We show that the total dissociation probability, the energy distribution, and the direction of ejection of the protons are very sensitive to the relative phase of the two radiations. A high degree of control may th us be achieved for the branching ratio between dissociation via bond-softening and above-threshold dissociation, in the realm of current experimental capabilities. PACS numbers: 33.80.Gj, 33 .80.Wz, 34.50.Rk Molecular dissociation in strong laser fields has been actively investigated in the past few years, both experimentally and theoretically. Several interesting processes have been found : (j) above-threshold dissociation (ATO) with stimulated emission as weil as multiphoton absorption occurring in the dissociation continuum; (ij) bond softening, [2,3] when a potential barrier in the dressed potential curves is sufficiently lowered by the radiative interaction that the initial vibration al level becornes unbound; (jji) suppression of dissociation, or stabilization due to temporary vibrational trapping in upper potential wells in the dressed potential curves [51. The relative importance of these three competing processes depends on the initial vibration al level, the laser intensity and wavelength, and the pulse duration . From the existing studies the A TO process appears to be the "Ioser," at least when starting from a mixture of vibrational levels, because dissociation by bond softening is very rapid as soon as the potential barrier can be overpassed.

Breakup of the H 2 molecule by xuv laser pulses: A time-dependent treatment in prolate spheroidal coordinates

Journal of Physics: Conference Series, 2012

We have carried out calculations of the triple-differential cross section for one-photon double ionization of molecular hydrogen for a central photon energy of 75 eV, using a fully ab initio, nonperturbative approach to solve the time-dependent Schrödinger equation in prolate spheroidal coordinates. The spatial coordinates ξ and η are discretized in a finite-element discrete-variable representation. The wave packet of the laser-driven two-electron system is propagated in time through an effective short iterative Lanczos method to simulate the double ionization of the hydrogen molecule. For both symmetric and asymmetric energy sharing, the present results agree to a satisfactory level with most earlier predictions for the absolute magnitude and the shape of the angular distributions. A notable exception, however, concerns the predictions of the recent time-independent calculations based on the exterior complex scaling method in prolate spheroidal coordinates [Phys. Rev. A 82, 023423 (2010)]. Extensive tests of the numerical implementation were performed, including the effect of truncating the Neumann expansion for the dielectronic interaction on the description of the initial bound state and the predicted cross sections. We observe that the dominant escape mode of the two photoelectrons dramatically depends upon the energy sharing. In the parallel geometry, when the ejected electrons are collected along the direction of the laser polarization axis, back-to-back escape is the dominant channel for strongly asymmetric energy sharing, while it is completely forbidden if the two electrons share the excess energy equally.