Attosecond electron wave packet interferometry

Remetter, T.; Johnsson, Per; Mauritsson, Johan; Varjú, Katalin; Ni, Y.; Lépine, F.; Gustafsson, E.; Kling, Matthias F.; Khan, J. I.; López-Martens, Rodrigo; Schafer, Kenneth J.; Vrakking, Marc J. J.; L’Huillier, Anne

doi:10.1038/nphys290

Cited by 228 publications

(189 citation statements)

References 25 publications

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“…Benefiting from the correlation between the electron launch time and its later-returning time, a similar pump-probe technique as in Ref. [41] may be a possible candidate in future experiments for exploring the quantum effect of closed classical orbits from a time-dependent viewpoint. An immediate application of the current theory would be the photodetachment of negative ions in a static electric field plus a strong oscillating electric field, where the averaged photodetachment rate can be detected as in Ref.…”

Section: Discussionmentioning

confidence: 99%

Closed-orbit theory for photodetachment in a time-dependent electric field

Yang

Robicheaux

2016

Phys. Rev. A

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The standard closed-orbit theory is extended for the photodetachment of negative ions in a timedependent electric field. The time-dependent photodetachment rate is specifically studied in the presence of a single-cycle terahertz pulse, based on exact quantum simulations and semiclassical analysis. We find that the photodetachment rate is unaffected by a weak terahertz field, but oscillates complicatedly when the terahertz pulse gets strong enough. Three types of closed classical orbits are identified for the photoelectron motion in a strong single-cycle terahertz pulse, and their connections with the oscillatory photodetachment rate are established quantitatively by generalizing the standard closed-orbit theory to a time-dependent form. By comparing the negative hydrogen and fluorine ions, both the in-phase and antiphase oscillations can be observed, depending on a simple geometry of the contributed closed classical orbits. On account of its generality, the presented theory provides an intuitive understanding from a time-dependent viewpoint for the photodetachment dynamics driven by an external electric field oscillating at low frequency.

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Section: Discussionmentioning

confidence: 99%

Closed-orbit theory for photodetachment in a time-dependent electric field

Yang

Robicheaux

2016

Phys. Rev. A

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“…Attosecond (as) pulses 1 provide access to these temporal regimes in different states of matter [2][3][4][5][6] . Nonlinear (NL) XUV processes constitute the ideal tool for the study of such dynamics.…”

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confidence: 99%

Extreme-ultraviolet pump–probe studies of one-femtosecond-scale electron dynamics

et al. 2011

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Ultrafast-dynamics studies and femtosecond-pulse metrology both rely on the nonlinear processes induced solely by an incident light pulse. Extending these approaches to the extreme-ultraviolet (XUV) spectral region would open up a new route to attosecond-scale dynamics. However, this has been hindered by the limited intensities available in coherent XUV continua. In the present work, we realized conditions at which simultaneous ejection of two bound electrons by two-XUVphoton absorption becomes more efficient than their removal one-by-one. In this regime we have succeeded in tracing atomic coherences evolving at the 1-fs scale with simultaneous determination of the average XUV-pulse duration. The rich and dense structure of the autoionizing manifold demonstrates the applicability of the approach to complex systems. This initiates the era of XUV-pump-XUV-probe experiments at the boundary between femto-and attosecond scales.A large variety of ultrafast phenomena, including electronic motion in atoms, molecules, condensed matter and plasmas, dynamic electron-electron correlations, charge migration, ultrafast dissociation and reaction processes, occur on the few-femtosecond to attosecond temporal scale. Attosecond (as) pulses 1 provide access to these temporal regimes in different states of matter [2][3][4][5][6] . Nonlinear (NL) XUV processes constitute the ideal tool for the study of such dynamics. Attosecond pulse trains 7-9 have reached intensities sufficient to induce two-XUV-photon processes [10][11][12][13][14] . However, isolated attosecond pulses, requisite for XUV-pump-XUV-probe experiments, have not yet attained the required parameters for an observable two-XUV-photon process. As a consequence, attosecond pulse metrology and time-domain applications have been widely based on infrared (IR)-XUV cross-correlation approaches, which entail assumptions for the analysis 15 .The present work succeeds for the first time in observing two-XUV-photon processes induced by energetic XUV continua, in part temporally confined in isolated pulses with durations on the order of 1 fs. These processes are in turn exploited in XUVpump-XUV-probe ultrafast evolving atomic coherences, as well as in determining the duration of the XUV bursts. A structured part of the single continuum of the xenon atom is excited by the first pulse, forming an electronic wave packet that undergoes rapid and complex motion before it decays. This evolution can be traced, thanks to the XUV parameters reached, at which a second pulse ejects a second electron before the first one leaves the atom carrying with it all the information on the temporal evolution of the system (coherence decay). Unconventionally, the two electrons leave the atom together and, thus, the doubly ionized Xe yield as a function of the delay between the two pulses carries the fingerprint of the wave packet motion and the XUV pulse duration. As the pulse duration and the decay The intense XUV radiation is generated by frequency upconversion of many-cycle high-peak-power laser fields...

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“…The availability of APT and IAP makes it capable of performing pump-probe experiments with APT or IAP as a pump pulse and infrared (IR) laser as a probe pulse (usually written as "APT+IR" or "IAP+IR") [59][60][61]. Such experiments have the advantage that the time delay between the APT (or IAP) and the IR can be controlled with high precision at the level of attoseconds.…”

Section: Spatiotemporal Dynamics Of Laser Pulsementioning

confidence: 99%

Theory of Nonlinear Propagation of High Harmonics Generated in a Gaseous Medium

Jin

2013

Springer Theses

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In this thesis, we establish the theoretical tools to investigate high-order harmonic generation (HHG) by intense infrared lasers in a gaseous medium. The macroscopic propagation of both the fundamental and the harmonic fields is taken into account by solving Maxwell's wave equations, while the single-atom (or single-molecule) response is obtained by quantitative rescattering theory. The initial spatial mode of the fundamental laser is assumed either a Gaussian or a truncated Bessel beam. On the examples of Ar, N 2 and CO 2 , we demonstrate that the available experimental HHG spectra with isotropic and aligned target media can be accurately reproduced theoretically even though the HHG spectra are sensitive to the experimental conditions. We show that the macroscopic HHG can be expressed as a product of a macroscopic wave packet and a photorecombination cross section, where the former depends on laser and experimental conditions while the latter is the property of the target only. The factorization makes it possible to retrieve the single-atom or single-molecule structure information from experimental HHG spectra. As for the multiple molecular orbital contribution in HHG, it causes the disappearance of the minimum in the HHG spectrum of aligned N 2 with the increase of laser intensity, and the position of minimum in HHG spectrum of aligned CO 2 depending on many factors is also attributed to it, which could explain why the minima observed in different laboratories may differ. For an important application of HHG as ultrashort light source, we show that measured continuous harmonic spectrum of Xe due to the reshaping of the fundamental laser field can be used to produce an isolated attosecond pulse by spectral and spatial filtering in the far field. For on-going application of using HHG to ionize aligned molecules, we present the photoelectron angular distribution from aligned N 2 and CO 2 in the laboratory frame, which can be compared directly with future experiments. demonstrate that the available experimental HHG spectra with isotropic and aligned target media can be accurately reproduced theoretically even though the HHG spectra are sensitive to the experimental conditions. We show that the macroscopic HHG can be expressed as a product of a macroscopic wave packet and a photorecombination cross section, where the former depends on laser and experimental conditions while the latter is the property of the target only. The factorization makes it possible to retrieve the single-atom or single-molecule structure information from experimental HHG spectra. As for the multiple molecular orbital contribution in HHG, it causes the disappearance of the minimum in the HHG spectrum of aligned N 2 with the increase of laser intensity, and the position of minimum in HHG spectrum of aligned CO 2 depending on many factors is also attributed to it, which could explain why the minima observed in different laboratories may differ. For an important application of HHG as ultrashort light source, we show that measured continu...

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Attosecond electron wave packet interferometry

Cited by 228 publications

References 25 publications

Closed-orbit theory for photodetachment in a time-dependent electric field

Closed-orbit theory for photodetachment in a time-dependent electric field

Extreme-ultraviolet pump–probe studies of one-femtosecond-scale electron dynamics

Theory of Nonlinear Propagation of High Harmonics Generated in a Gaseous Medium

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