Photon-recoil imaging: Expanding the view of nonlinear x-ray physics.

Addressing the ultrafast coherent evolution of electronic wave functions has long been a goal of nonlinear x-ray physics. A first step toward this goal is the investigation of stimulated x-ray Raman scattering (SXRS) using intense pulses from an x-ray free-electron laser. Earlier SXRS experiments relied on signal amplification during pulse propagation through dense resonant media. By contrast, our method reveals the fundamental process in which photons from the primary radiation source directly interact with a single atom. We introduce an experimental protocol in which scattered neutral atoms rather than scattered photons are detected. We present SXRS measurements at the neon K edge and a quantitative theoretical analysis. The method should become a powerful tool in the exploration of nonlinear x-ray physics.

Frustrated tunnel ionization of noble gas dimers with Rydberg-electron shakeoff by electron charge oscillation.

Strong field single ionization of homo- and heteronuclear noble gas dimers with ultrashort infrared laser pulses is experimentally investigated. A pronounced photoelectron yield maximum is found for dimers in the momentum range |p|≤0.1 a.u. which is absent for the corresponding monomer. This yield enhancement can be attributed to a new two-step strong field ionization mechanism active only in the dimers. In the first step, frustrated tunnel ionization at one of the atomic centers populates Rydberg states, which then become ionized in a second step through charge oscillation within the dimer ion core.

Acceleration of neutral atoms in strong short-pulse laser fields.

A charged particle exposed to an oscillating electric field experiences a force proportional to the cycle-averaged intensity gradient. This so-called ponderomotive force plays a major part in a variety of physical situations such as Paul traps for charged particles, electron diffraction in strong (standing) laser fields (the Kapitza-Dirac effect) and laser-based particle acceleration. Comparably weak forces on neutral atoms in inhomogeneous light fields may arise from the dynamical polarization of an atom; these are physically similar to the cycle-averaged forces. Here we observe previously unconsidered extremely strong kinematic forces on neutral atoms in short-pulse laser fields. We identify the ponderomotive force on electrons as the driving mechanism, leading to ultrastrong acceleration of neutral atoms with a magnitude as high as approximately 10(14) times the Earth's gravitational acceleration, g. To our knowledge, this is by far the highest observed acceleration on neutral atoms in external fields and may lead to new applications in both fundamental and applied physics.

Strong laser field fragmentation of H2: Coulomb explosion without double ionization.

We observe fragmentation of H2 molecules exposed to strong laser fields into excited neutral atoms. The measured excited neutral fragment spectrum resembles the ionic fragmentation spectrum including peaks due to bond softening and Coulomb explosion. To explain the occurrence of excited neutral fragments and their high kinetic energy, we argue that the recently investigated phenomenon of frustrated tunnel ionization is also at work in the neutralization of H+ ions into excited H atoms. In this process the tunneled electron does not gain enough drift energy from the laser field to escape the Coulomb potential and is recaptured. Calculation of classical trajectories as well as a correlated detection measurement of neutral excited H and H+ ions support the mechanism.

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.

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.

Rescattering of ultralow-energy electrons for single ionization of Ne in the tunneling regime.

Electron emission for single ionization of Ne by 25 fs, 1.0 PW/cm(2) laser pulses at 800 nm has been investigated in a kinematically complete experiment using a "reaction microscope." Mapping the complete final state momentum space with high resolution, a distinct local minimum is observed at P(e parallel )=0, where P(e parallel ) is the electron momentum parallel to the laser polarization. Whereas tunneling theory predicts a maximum at zero momentum, our findings are in good agreement with recent semiclassical predictions which were interpreted to be due to "recollision."

Coincident fragment detection in strong field photoionization and dissociation of H2.

Electron-ion momentum spectroscopy is used to investigate the correlated electronic and nuclear motion in fragmentation of H2 in 4 x 10(14) W/cm(2), 25 fs laser pulses at 795 nm. Reaction channel dependent photoelectron spectra indicate that besides the main, stepwise H2 ionization H2(+) dissociation mechanism resulting in the products H(1s) + H(+) + e(-) a second new mechanism has to be assumed. The momentum distribution of H(+) ions in the dissociation channels H(1s) + H(+) + e(-) and 2H(+) + 2e(-) is found to be independent of the kinetic energy of the photoelectrons.

Separation of recollision mechanisms in nonsequential strong field double ionization of Ar: the role of excitation tunneling.

Vector momentum distributions of two electrons created in double ionization of Ar by 25 fs, 0.25 PW/cm(2) laser pulses at 795 nm have been measured using a "reaction microscope." At this intensity, where nonsequential ionization dominates, distinct correlation patterns are observed in the two-electron momentum distributions. A kinematical analysis of these spectra within the classical "recollision model" revealed an (e,2e)-like process and excitation with subsequent tunneling of the second electron as two different ionization mechanisms. This allows a qualitative separation of the two mechanisms demonstrating that excitation-tunneling is the dominant contribution to the total double ionization yield.

Non-sequential double ionization of Ne in intense laser pulses: a coincidence experiment.

The dynamics of Neon double ionization by 25 fs, 1.0 PW/cm 2 laser pulses at 795 nm has been studied in a many particle coincidence experiment. The momentum vectors of all ejected atomic fragments (electrons and ions) have been measured using combined electron and recoil-ion momentum spectroscopy. Electron emission spectra for double and single ionization will be discussed. In both processes the mean electron energies differ considerably and high energetic electrons with energies of more than 120 eV have been observed for double ionization. The experimental results are in qualitative agreement with the rescattering model.

Momentum distributions of ne(n+) ions created by an intense ultrashort laser pulse

Vector momentum distributions of Ne(n+) (n = 1,2,3) ions created by 30 fs, approximately 1 PW/cm(2) laser pulses at 795 nm have been measured using recoil-ion momentum spectroscopy. Distinct maxima along the light polarization axis are observed at 4.0 and 7.5 a.u. for Ne2+ and Ne3+ production, respectively. Hence, mechanisms based on an instantaneous release of two (or more) electrons can be ruled out as a dominant contribution to nonsequential strong-field multiple ionization. The positions of the maxima are in accord with kinematical constraints set by the classical "rescattering model."

Routes to nonsequential double ionization

A method is proposed for the calculation of the S matrix for many-electron processes in intense-laser atom physics, in close analogy to the strong-field approximation for one-electron processes. Given a scenario of how some process evolves, corresponding approximations to the classical action are made which allow for the evaluation of the quantum-mechanical S matrix. The method is applied to the distribution of the total electronic momentum in nonsequential double ionization, and the results are compared to recent measurements. Good agreement is obtained for neon for a rescattering scenario. There is no comparable agreement for helium and argon, and possible alternative scenarios are discussed.