18 research outputs found

    Probing time-ordering in two-photon double ionization of helium on the attosecond time scale

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    We show that time ordering underlying time-dependent quantum dynamics is a physical observable accessible by attosecond streaking. We demonstrate the extraction of time ordering for the prototypical case of time-resolved two-photon double ionization (TPDI) of helium by an attosecond XUV pulse. The Eisenbud-Wigner-Smith time delay for the emission of a two-electron wavepacket and the time interval between subsequent emission events can be unambiguously determined by attosecond streaking. The delay between the two emission events sensitively depends on the energy, pulse duration, and angular distribution of the emitted electron pair. Our fully-dimensional ab-initio quantum mechanical simulations provide benchmark data for experimentally accessible observables.Comment: 8 pages, 5 figures; revised version, added appendi

    Photoionization of helium by attosecond pulses: extraction of spectra from correlated wave functions

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    We investigate the photoionization spectrum of helium by attosecond XUV pulses both in the spectral region of doubly excited resonances as well as above the double ionization threshold. In order to probe for convergence, we compare three techniques to extract photoelectron spectra from the wavepacket resulting from the integration of the time-dependent Schroedinger equation in a finite-element discrete variable representation basis. These techniques are: projection on products of hydrogenic bound and continuum states, projection onto multi-channel scattering states computed in a B-spline close-coupling basis, and a technique based on exterior complex scaling (ECS) implemented in the same basis used for the time propagation. These methods allow to monitor the population of continuum states in wavepackets created with ultrashort pulses in different regimes. Applications include photo cross sections and anisotropy parameters in the spectral region of doubly excited resonances, time-resolved photoexcitation of autoionizing resonances in an attosecond pump-probe setting, and the energy and angular distribution of correlated wavepackets for two-photon double ionization.Comment: 19 pages, 12 figure

    Attosecond streaking of Cohen-Fano interferences in the photoionization of H2+_2^+

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    We present the first numerical simulation of the time delay in the photoionization of the simplest diatomic molecule H2+_2^+ as observed by attosecond streaking. We show that the strong variation of the Eisenbud-Wigner-Smith time delay as a function of energy and emission angle becomes observable in the streaking time shift provided laser field-induced components are accounted for. The strongly enhanced photoemission time shifts are traced to destructive Cohen-Fano (or two-center) interferences. Signatures of these interferences in the streaking trace are shown to be enhanced when the ionic fragments are detected in coincidence

    Attosecond streaking of correlated two-electron transitions in helium

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    We present fully ab initio simulations of attosecond streaking for ionization of helium accompanied by shake-up of the second electron. This process represents a prototypical case for strongly correlated electron dynamics on the attosecond timescale. We show that streaking spectroscopy can provide detailed information on the Eisenbud-Wigner-Smith time delay as well as on the infrared field dressing of both bound and continuum states. We find a novel contribution to the streaking delay that stems from the interplay of electron-electron and infrared-field interactions in the exit channel. We quantify all the contributions with attosecond precision and provide a benchmark for future experiments.Comment: 5 pages, 4 figure

    Ionization delays in few-cycle-pulse multiphoton quantum-beat spectroscopy in helium

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    We explore quantum beats in the photoelectron signal produced when a bound electron wave packet created by an isolated attosecond pulse is ionized by a delayed, few-cycle infrared pulse. Our calculations for helium atoms show that the broad bandwidth of the few-cycle pulse creates spectrally overlapping photoelectron peaks that result from one-, two-, or three-photon ionization processes. The beat signals can, in principle, be interferometrically resolved with high resolution, giving access to the relative phase between different multiphoton ionization pathways. For few-cycle near-infrared fields the relative spectral phases can be extracted over a large energy region, and dynamical information becomes available. We find that multiphoton ionization is temporally shifted with respect to one-photon ionization by several hundred attoseconds. Our results also reveal the impact of depletion and resonant pathways on the phase of the quantum beats
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