Real-time observation of valence electron motion

Goulielmakis, Eleftherios; Loh, Zhi-Heng; Wirth, Adrian; Santra, Robin; Rohringer, Nina; Yakovlev, Vladislav S.; Zherebtsov, Sergey; Pfeifer, Thomas; Azzeer, Abdallah M.; Kling, Matthias F.; Leone, Stephen R.; Krausz, Ferenc

doi:10.1038/nature09212

Cited by 1,155 publications

(1,032 citation statements)

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“…However, the process is insensitive to the coherence between the two states. This differs from other recently introduced methods, like attosecond transient absorption [7] and strong-field ionization [31] to probe electronic dynamics. Carbon dioxide is an instructive model system to understand multielectron effects in HHS.…”

Section: Probing Electronic Dynamicsmentioning

confidence: 84%

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High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

Wörner

2011

Chimia

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The principles of high-harmonic spectroscopy (HHS) are illustrated using two recent examples from the literature. The method can be applied as a probe to measure the evolution of the electronic structure of a molecule during a chemical reaction on the femtosecond time scale. Alternatively, it can be used as a comprehensive method unifying pump and probe steps into a single laser cycle to measure electronic dynamics on the at to second time scale.

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Section: Probing Electronic Dynamicsmentioning

confidence: 84%

“…The last few years have seen first successes in the observation of electronic dynamics on this time scale. [3][4][5][6][7] These techniques will enable a new experimental access to electronic structure and electron correlation, which is one of the most challenging problems in chemistry and physics.…”

Section: Introductionmentioning

confidence: 99%

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

Wörner

2011

Chimia

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“…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]. The images (Fig.…”

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confidence: 99%

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

Ott

Kaldun

Argenti

et al. 2014

Nature

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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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“…On the one hand, ultrahigh light intensities provided by multi-terawatt femtosecond lasers can be used to drive collective electron motion in plasmas up to the 0.1-1 gigaelectronvolt energy range [1], opening the way to very compact laser-based particle accelerators for nuclear and medical applications [2]. On the other hand, controlled few-cycle light waves can be used at moderate intensities to drive and probe the attosecond dynamics of few-electron motion in atoms [3,4,5,6], molecules [7,8] and condensed matter [9,10] -with typical energies * These authors contributed equally to this work. …”

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confidence: 99%

Attosecond control of collective electron motion in plasmas

et al. 2012

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Today, light fields of controlled and measured waveform can be used to guide electron motion in atoms and molecules with attosecond precision. Here, we demonstrate attosecond control of collective electron motion in plasmas driven by extreme intensity (≈ 10 18 W/cm 2 ) light fields.Controlled few-cycle near-infrared light waves are tightly focused at the interface between vacuum and a solid-density plasma, where they launch and guide subcycle motion of electrons from the plasma with characteristic energies in the multi-kiloelectronvolt range -two orders of magnitude more than what has been achieved so far in atoms and molecules. Basic spectroscopy of the coherent extreme ultraviolet radiation emerging from the light-plasma interaction allows us to probe this collective motion of charge with sub-100-attosecond resolution. This is an important step towards attosecond control of charge dynamics in laser-driven plasma experiments.Two major trends can nowadays be identified in the interaction of ultrashort laser pulses with matter. On the one hand, ultrahigh light intensities provided by multi-terawatt femtosecond lasers can be used to drive collective electron motion in plasmas up to the 0.1-1 gigaelectronvolt energy range [1], opening the way to very compact laser-based particle accelerators for nuclear and medical applications [2]. On the other hand, controlled few-cycle light waves can be used at moderate intensities to drive and probe the attosecond dynamics of few-electron motion in atoms [3,4,5,6], molecules [7,8] and condensed matter [9,10] -with typical energies * These authors contributed equally to this work. 1ranging between tens to a few hundred electronvolts [11]. Merging these two trends, i.e. using tailored waveforms of extreme intensity light to steer the collective motion of high-energy plasma electrons, will open brand new perspectives for imaging ultrafast charge dynamics during extreme intensity laser-plasma interactions. First experiments have already highlighted the need for waveform control when trying to reproducibly guide attosecond electronic processes in plasmas with intense few-cycle light fields [12]. For the first time, we use fully controlled few-cycle near-infrared (NIR) light fields of extreme intensity (10 18 W/cm 2 ) to reproducibly launch and probe collective electron motion at the interface between vacuum and a solid-density plasma with attosecond precision (Fig. 1a-b). Light-driven plasma mirrorsWhen an intense femtosecond laser pulse interacts with a solid, its rising edge strongly ionizes the surface atoms, creating a layer of plasma with near-solid electronic density (∼ 10 23 cm −3 ), which becomes highly reflectivea so-called plasma mirror -for light at wavelengths greater than a few tens of nanometers [13,14,15,16,17].During the interaction with the pulse, the plasma layer can only expand by a small fraction of the optical laser wavelength, λL, which leads to the formation of a very sharp interface with vacuum extending over a distance λL (Fig. 1b), typically of the order o...

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Real-time observation of valence electron motion

Cited by 1,155 publications

References 30 publications

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

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

Attosecond control of collective electron motion in plasmas

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