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We report on a kinematically complete measurement of double ionization of helium by a single 1100 eV circularly polarized photon. By exploiting dipole selection rules in the two-electron continuum state, we observed the angular emission pattern of electrons originating from a pure quadrupole transition. Our fully differential experimental data and companion ab initio nonperturbative theory show the separation of dipole and quadrupole contributions to photo-double-ionization and provide new insight into the nature of the quasifree mechanism.
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Single-photon laser-enabled Auger decay (spLEAD) is predicted theoretically [B. Cooper and V. Averbukh, Phys. Rev. Lett. 111, 083004 (2013)PRLTAO0031-900710.1103/PhysRevLett.111.083004] and here we report its first experimental observation in neon. Using coherent, bichromatic free-electron laser pulses, we detect the process and coherently control the angular distribution of the emitted electrons by varying the phase difference between the two laser fields. Since spLEAD is highly sensitive to electron correlation, this is a promising method for probing both correlation and ultrafast hole migration in more complex systems.
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We combine IR pump and XUV probe laser pulses to visualize the Kramers-Henneberger (KH) state of the potassium atom. We demonstrate that ionization of such an atom exhibits some molecular-like features such as low order interference maxima in photoelectron momentum spectra. The locations of these maxima allow to estimate spatial dimensions of the KH atom and can be used for accurate calibration of high intensity laser fields. At the same time, we show that an analogy between the KH atom and a homo-nuclear diatomic molecule cannot be extended too far. In particular, higher order interference maxima are very difficult to observe in the case of the KH state. We attribute this to a particular structure of the KH potential which does not confine electron motion to a well-defined potential well unlike in real diatomic molecules.
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We analyze the time delay between emission of photoelectrons from the outer valence ns and np subshells in noble gas atoms following absorption of an attosecond extreme ultraviolet pulse. Various processes such as elastic scattering of the photoelectron on the parent ion and many-electron correlation affect the apparent "time zero" when the photoelectron leaves the atom. This qualitatively explains the time delay between photoemission from the 2s and 2p subshells of Ne as determined experimentally by attosecond streaking [Science 328, 1658 (2010)]. However, with our extensive numerical modeling, we were only able to account for less than half of the measured time delay of 21 ± 5 as. We argue that the extreme ultraviolet pulse alone cannot produce such a large time delay and it is the streaking IR field that is most likely responsible for this effect.
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The original version of this Article contained an error in the fifth sentence of the first paragraph of the 'Application on H2' section of the Results, which incorrectly read 'The role of electron correlation is quite apparent in this presentation: Fig. 1a is empty for the uncorrelated Hartree-Fock wave function, since projection of the latter wave function onto the 2pσu orbital is exactly zero, while this is not the case for the fully correlated wave function (Fig. 1d); also, Fig. 1b, c for the uncorrelated description are identical, while Fig. 1e, f for the correlated case are significantly different.' The correct version replaces 'Fig. 1e, f' with 'Fig. 2e and f'.
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The toolbox for imaging molecules is well-equipped today. Some techniques visualize the geometrical structure, others the electron density or electron orbitals. Molecules are many-body systems for which the correlation between the constituents is decisive and the spatial and the momentum distribution of one electron depends on those of the other electrons and the nuclei. Such correlations have escaped direct observation by imaging techniques so far. Here, we implement an imaging scheme which visualizes correlations between electrons by coincident detection of the reaction fragments after high energy photofragmentation. With this technique, we examine the H2 two-electron wave function in which electron-electron correlation beyond the mean-field level is prominent. We visualize the dependence of the wave function on the internuclear distance. High energy photoelectrons are shown to be a powerful tool for molecular imaging. Our study paves the way for future time resolved correlation imaging at FELs and laser based X-ray sources.
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We study transverse electron momentum distribution in strong field atomic ionization driven by laser pulses with varying ellipticity. We show, both experimentally and theoretically, that the transverse electron momentum distribution in the tunneling and over the barrier ionization regimes evolves in a qualitatively different way when the ellipticity parameter describing polarization state of the driving laser pulse increases.
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This work describes the first observations of the ionisation of neon in a metastable atomic state utilising a strong-field, few-cycle light pulse. We compare the observations to theoretical predictions based on the Ammosov-Delone-Krainov (ADK) theory and a solution to the time-dependent Schrödinger equation (TDSE). The TDSE provides better agreement with the experimental data than the ADK theory. We optically pump the target atomic species and measure the ionisation rate as the a function of different steady-state populations in the fine structure of the target state which shows significant ionisation rate dependence on populations of spin-polarised states. The physical mechanism for this effect is unknown.
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Double ionization of the helium atom by slow electron impact (E(0)=106 eV) is studied in a kinematically complete experiment. Because of a low excess energy E(exc)=27 eV above the double ionization threshold, a strongly correlated three-electron continuum is realized. This is demonstrated by measuring and calculating the fully differential cross sections for equal energy sharing of the final-state electrons. While the electron emission is dominated by a strong Coulomb repulsion, also signatures of more complex dynamics of the full four-body system are identified.
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Simultaneous ionization and excitation of helium atoms by 500 eV electron impact is observed by a triple coincidence of an ionized slow electron, the recoiling He+ ion, and the radiated vacuum ultraviolet photon (lambda< or =30.4 nm). Kinematically complete differential cross sections are presented for the He+(2p)2P final ionic state, demonstrating the feasibility of a quantum mechanically complete experiment. The experimental data are compared to predictions from state-of-the-art numerical calculations. For large momentum transfers, a first-order treatment of the projectile-target interaction can reproduce the experimental angular dependence, but a second-order treatment is required to obtain consistent magnitudes.
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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.