While, at the same time, the correlated momenta of the entangled electron pair continue to exhibit quantum interference.

Using a simple model of strong-field ionization of atoms that generalizes the well-known 3-step model from 1D to 3D, we show that the experimental photoelectron angular distributions resulting from laser ionization of xenon and argon display prominent structures that correspond to electrons that pass by their parent ion more than once before strongly scattering. The shape of these structures can be associated with the specific number of times the electron is driven past its parent ion in the laser field before scattering. Furthermore, a careful analysis of the cutoff energy of the structures allows us to experimentally measure the distance between the electron and ion at the moment of tunnel ionization. This work provides new physical insight into how atoms ionize in strong laser fields and has implications for further efforts to extract atomic and molecular dynamics from strong-field physics. DOI: 10.1103/PhysRevLett.109.073004 PACS numbers: 32.80.Fb, 32.80.Rm, 34.80.Qb When an atom or molecule is illuminated with a moderately intense femtosecond laser field ($ 10 14 W=cm 2 ), an electron wave packet will tunnel ionize and accelerate in the field before being turned around by the field and returning to the parent ion. The returning electron can either recombine with the parent ion, releasing its kinetic energy as a high-energy photon [1-3], or can elastically scatter from the potential of the ion. The photons and electrons generated by these strong-field processes have the potential to probe the dynamic structure of molecules and materials on the subnanometer length scale and femtosecond-to-attosecond time scale. Several recent papers have suggested that structures seen in angledependent photoelectron spectra may be useful for determining time-resolved molecular structures [4], characterizing attosecond electron wave packets [5], and studying the dynamics of electron wave packet propagation [6]. However, despite extensive analyses [7][8][9][10][11], many features observed in angle-resolved photoelectron spectra still lack a simple physical explanation.The recent development of midinfrared (mid-IR) femtosecond lasers [12] and angle-resolved detection schemes [13] has enabled new advances in visualizing strong-field physics. Electrons that are ionized in a mid-IR laser field reach higher velocities because of the larger ponderomotive energy, given by U P / I 2 , where I is the intensity and is the wavelength. The possibility of harnessing the high-energy electrons that are first ionized and then driven back to a molecule by a strong laser field has inspired several theoretical and experimental efforts to use strongfield ionization to probe molecular structure [4,[14][15][16]. Recently, Huismans and co-workers [17] used 7 m mid-IR lasers, in combination with angle-resolved detection, to observe angular interference structures in the photoelectron spectra. They presented a theoretical model that explains these structures based on the difference in the phase between two different paths that electrons can take to...

Two-color (800 and 400 nm) short (45 fs) linearly polarized pulses are used to ionize and dissociate D2 into a neutral deuterium atom and a deuteron. The yields and energies of the ions are measured left and right along the polarization vector. As the relative phase of the two colors is varied, strong yield asymmetries are found in the ion-energy regions traditionally identified as bond softening, above-threshold dissociation and rescattering. The asymmetries in these regions are quite different. A model based on the dynamic coupling by the laser field of the gerade and ungerade states in the molecular ion accounts for many of the observed features.

We have measured coincident ion pairs produced in the Coulomb explosion of H2 by 8-30 fs laser pulses at different laser intensities. We show how the Coulomb explosion of H2 can be experimentally controlled by tuning the appropriate pulse duration and laser intensity. For laser pulses less than 15 fs, we found that the rescattering-induced Coulomb explosion is dominated by first-return recollisions, while for longer pulses and at the proper laser intensity, the third return can be made to be the major one. Additionally, by choosing suitable pulse duration and laser intensity, we show H2 Coulomb explosion proceeding through three distinct processes that are simultaneously observable, each exhibiting different characteristics and revealing distinctive time information about the H2 evolution in the laser pulse.

The direct observation of molecular dynamics initiated by x-rays has been hindered to date by the lack of bright femtosecond sources of short-wavelength light. We used soft x-ray beams generated by high-harmonic upconversion of a femtosecond laser to photoionize a nitrogen molecule, creating highly excited molecular cations. A strong infrared pulse was then used to probe the ultrafast electronic and nuclear dynamics as the molecule exploded. We found that substantial fragmentation occurs through an electron-shakeup process, in which a second electron is simultaneously excited during the soft x-ray photoionization process. During fragmentation, the molecular potential seen by the electron changes rapidly from nearly spherically symmetric to a two-center molecular potential. Our approach can capture in real time and with angstrom resolution the influence of ionizing radiation on a range of molecular systems, probing dynamics that are inaccessible with the use of other techniques.

We demonstrate an experimental control of electron localization in deuterium molecular ions created and dissociated by the combined action of an attosecond pulse train and a many-cycle infrared (IR) pulse. The attosecond pulse train is synthesized using both even and odd high order harmonics of the driving IR frequency so that it can strobe the IR field once per IR cycle. An asymmetric ejection of the deuterium ions oscillates with the full IR period when the APT-IR time-delay is scanned. The observed control is due to the creation of a coherent superposition of 1s sigma{g} and 2p sigma{u} states via interference between one-photon and two-photon dissociation channels.

We have measured momentum-space images of low-energy electrons generated by the interaction of short intense laser pulses with argon atoms at high intensities. We have done this over a wavelength range from 400 to 800 nm. The spectra show considerable structure in both the energy and angular distributions of the electrons. Some, but not all, energy features can be identified as multiphoton resonances. The angular structure shows a regularity which transcends the resonant structure and may be due instead to diffraction. The complexity of the results defies easy model-dependent interpretations and invites full solutions to Schrödinger's equation for these systems.

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