Observation of a Train of Attosecond Pulses from High Harmonic Generation

Paul, P.; Toma, E. S.; Breger, P.; Mullot, G.; Augé, F.; Balcou, Philippe; Müller, H. G.; Agostini, Pierre

doi:10.1126/science.1059413

Cited by 2,429 publications

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“…4a, showing no significant changes in the absorbance spectra. This is a direct consequence of the well-known 23 phase locking of the attosecond pulses to the half cycles of the generating intense VIS pulses. In the energy domain, this corresponds to a well-defined coherent excitation spectrum over a broadband spectral range.…”

Section: Methodsmentioning

confidence: 96%

“…1a; Methods -Experimental Apparatus Details‖) consisting of a XUV source chamber, refocusing and time-delay chamber and a target chamber followed by a highresolution (= 0.01 nm, corresponding to 20 meV near ~60 eV) XUV spectrometer. Trains of few attosecond XUV pulses with ~600 as duration are generated by the intrinsically phase locked 23 broadband harmonics in the relevant region of 60-65 eV by high-order harmonic generation (HHG) in a gas cell filled with neon (~100 mbar). The generated XUV pulses then co-propagate with their intense driver pulse and impinge at 15-degree grazing-incidence angle on a two-component split mirror.…”

Section: Methods Summarymentioning

confidence: 99%

“…5. For the definition of the attosecond pulse and its time of arrival with respect to the (generating) VIS laser pulse we used the coherence (phase locking) between two harmonics, which has been confirmed numerous times to be present in high-harmonic generation since its first direct measurement via interferometric twophoton photoelectron spectroscopy 23 . Assuming this phase locking of two harmonics in the energy region 60-64 eV produced the attosecond pulse trains in the model simulation, and also defines the individual attosecond pulse duration to ~600 as, as stated in the Methods Summary section of the main text.…”

Section: Methodsmentioning

confidence: 99%

“…Due to the well-defined spectral coherence (i.e. phase locking 23 ) present in a highharmonic spectrum, the observation of a well-defined phase evolution υ(t) is possible 24 even in the absence of carrier-envelope-phase stabilization and without knowing the number of attosecond pulses in our few-cycle generated attosecond-pulse train (Methods -Effects of the Attosecond Pules Configuration and the Carrier Envelope Phase‖; Extended Data Figs. [4][5][6].…”

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confidence: 99%

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Reconstruction and control of a time-dependent two-electron wave packet

Ott

Kaldun

Argenti

et al. 2014

Nature

272

218

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Esta es la versión de autor del artículo publicado en: This is an author produced version of a paper published in: The concerted motion of two or more bound electrons governs atomic 1 and molecular 2,3 non-equilibrium processes and chemical reactions. It is thus a long-standing scientific dream to measure and control the dynamics of two bound and correlated electrons in the quantum regime. At least two active electrons and a nucleus are required to address such quantum three-body problem 4 for which analytical solutions do not exist, a condition that is met in the helium atom. While attosecond dynamics were previously observed for singleactive electron/hole cases 5-7 , such time-resolved observation of two-electron motion thus far remained an unaccomplished challenge. Here, we measure a 1.2-femtosecond quantum beat among low-lying doubly-excited states in helium and use it to reconstruct a correlated two-electron wave packet. Our experimental method combines attosecond transientabsorption spectroscopy 5,7-9 at unprecedented high spectral resolution (20 meV s.d. near 60 eV) with an intensity-tuneable visible laser field to couple 10-12 the quantum states from the weak-field to the strong-coupling regime. Employing the Fano resonance as a phasesensitive quantum interferometer 13 , we demonstrate the coherent control of two correlated electrons, which form the basis of most covalent molecular bonds in nature. As we show, such multi-dimensional spectroscopy experiments provide benchmark data for testing fundamental few-body quantum-dynamics theory. They also light a route for site-specific measurement and control of metastable electronic transition states that are at the heart of fundamental reactions in chemistry and biology.Electrons are bound to atoms and molecules by the Coulomb force of the nuclei. Moving between atoms, they form the basis of the molecular bond. The same Coulomb force, however, acts repulsively between the electrons. This electron-electron interaction represents a major challenge in the understanding and modelling of atomic and molecular states, their structure and in particular their dynamics 2,3,14 . Here, we focus on the 1 P sp 2,n+ series 15 of doubly-excited states in helium below the N = 2 ionization threshold. They are excited by a single-photon transition from the 1 S 1s 2 ground state by the promotion of both electrons to at least principal quantum number n = 2. The states autoionize due to electron-electron interaction and their spectroscopic signature manifests as asymmetric non-Lorentzian line shapes. The latter were first observed in the 1930s 16 and attributed 17 , by Ugo Fano, to the quantum interference of bound states with the continuum to which they are coupled (Fig. 1c,d). The coupling is described by the configuration interaction V CI with the single-ionization continuum |1s,p, where one electron is in the 1s ground state and the other one is in the continuum with kinetic energy . The magnitude of V CI determines the lifetimes of the transiently bound states. In our case,...

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Section: Methodsmentioning

confidence: 96%

Section: Methods Summarymentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

mentioning

confidence: 99%

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Reconstruction and control of a time-dependent two-electron wave packet

Ott

Kaldun

Argenti

et al. 2014

Nature

272

218

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“…The combined nuclear-electron wave packet dynamics of CO 2 has been studied for short (<200 fs) pulses using the field-following time-dependent adiabatic state approach. [34][35][36] In the few-cycle pulse regime for CO 2 , the electron dynamics are the main contributor to any excitation processes since there is not sufficient time for the nuclear motion to occur. The electron dynamics for pulses on the order of a few cycles and the effect of CEP have not been studied for CO 2 .…”

Section: Introductionmentioning

confidence: 99%

Numerical Bound State Electron Dynamics of Carbon Dioxide in the Strong-Field Regime

Smith

Romanov

et al. 2010

J. Phys. Chem. A

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Time-dependent Hartree-Fock simulations for a linear triatomic molecule (CO 2 ) interacting with a short IR (1.63 eV) three-cycle pulse reveal that the carrier-envelope shape and phase are the essential field parameters determining the bound state electron dynamics during and after the laser-molecule interaction. Analysis of the induced dipole oscillation reveals that the envelope shape (Gaussian or trapezoidal) controls the excited state population distribution. Varying the carrier envelope phase for each of the two pulse envelope shapes considerably changes the excited state populations. Increasing the electric field amplitude alters the relative populations of the excited states, generally exciting higher states. A windowed Fourier transform analysis of the dipole evolution during the laser pulse reveals the dynamics of state excitation and in particular state coupling as the laser intensity increases.

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Ultrashort‐pulse Phenomena

Powers

Spence

Tang

2004

Digital Encyclopedia of Applied Physics

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Ultrashort‐pulse phenomena are generally processes that occur on the subpicosecond to femtosecond time scale. The availability of lasers that generate ultrashort optical pulses has made possible the study of effects and processes that occur on ultrashort time scales. These measurements have led to a more fundamental understanding of processes in fields ranging from chemical kinetics to semiconductor physics. The high peak powers attainable with ultrashort‐pulse lasers has also led to new applications such as soft X‐ray generation and multiphoton microscopy. In this article, we review the generation, characterization, and a few of the applications of ultrashort optical pulses. We briefly introduce these topics with the goal of presenting an overview of the fundamental ideas. An extensive list of references is provided for each topic to give a starting point for further research.

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Observation of a Train of Attosecond Pulses from High Harmonic Generation

Cited by 2,429 publications

References 19 publications

Reconstruction and control of a time-dependent two-electron wave packet

Reconstruction and control of a time-dependent two-electron wave packet

Numerical Bound State Electron Dynamics of Carbon Dioxide in the Strong-Field Regime

Ultrashort‐pulse Phenomena

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