International audienceA strong laser field may tunnel ionize a molecule from several orbitals simultaneously, forming an attosecond electron–hole wavepacket. Both temporal and spatial information on this wavepacket can be obtained through the coherent soft X-ray emission resulting from the laser-driven recollision of the liberated electron with the core. By characterizing the emission from aligned N 2 molecules, we demonstrate the attosecond contributions of the two highest occupied molecular orbitals. We determine conditions where they are disentangled in the real and imaginary parts of the emission dipole moment. This allows us to carry out a tomographic reconstruction of both orbitals with angstrom spatial resolution. Their coherent superposition provides experimental images of the attosecond wavepacket created in the ionization process. Our results open the prospect of imaging ultrafast intramolecular dynamics combining attosecond and angstrom resolutions

Esta es la versión de autor del artículo publicado en: This is an author produced version of a paper published in:Science 354(6313) (2016): 734-738 DOI: http://dx.doi.org/10.1126/science.aah5188 Copyright: © 2016 American Association for the Advancement of ScienceEl acceso a la versión del editor puede requerir la suscripción del recurso Access to the published version may require subscription However, the rapidity of electron dynamics on the attosecond timescale has precluded their complete measurement in the time domain. Here, we demonstrate that spectrally-resolved electron interferometry reveals the amplitude and phase of a photoelectron wavepacket created through a Fano autoionizing resonance in helium. Replicas obtained by two-photon transitions interfere with reference wavepackets formed through smooth continua, allowing the full temporal reconstruction, purely from experimental data, of the resonant wavepacket released in the continuum. This in turn resolves the buildup of the autoionizing resonance on attosecond timescale. Our results, in excellent agreement with ab initio time-dependent calculations, raise prospects for both detailed investigations of ultrafast photoemission dynamics governed by electron correlation, as well as coherent control over structured electron wave-packets.One Sentence Summary: By monitoring the decay of an excited atom in real time, we reconstruct how photoelectron wavepackets are born and morph into asymmetric Fano profiles. Main Text:Tracking electronic dynamics on the attosecond (as) timescale and Ångström (Å) lengthscale is a key to understanding and controlling the quantum mechanical underpinnings of physical and chemical transformations (1). One of the most fundamental electronic processes in this context is photoelectron emission, the dynamics of which are fully encoded in the released electron wavepacket (EWP) and the final ionic state. The development of broadband coherent sources of attosecond pulses has opened the possibility of investigating these dynamics with attosecond resolution. On such a short timescale, few techniques (2-5) are able to provide access to both spectral amplitude and phase. The spectral derivative of the phase, the group delay, is a practical quantity for describing general wavepacket properties reflecting the ionization dynamics.

International audienceCircular dichroism in the extreme ultraviolet range is broadly used as a sensitive structural probe of matter, from the molecular photoionization of chiral species1, 2, 3 to the magnetic properties of solids4. Extending such techniques to the dynamical regime has been a long-standing quest of solid-state physics and physical chemistry, and was only achieved very recently5 thanks to the development of femtosecond circular extreme ultraviolet sources. Only a few large facilities, such as femtosliced synchrotrons6, 7 or free-electron lasers8, are currently able to produce such pulses. Here, we propose a new compact and accessible alternative solution: resonant high-order harmonic generation of an elliptical laser pulse. We show that this process, based on a simple optical set-up, delivers bright, coherent, ultrashort, quasi-circular pulses in the extreme ultraviolet. We use this source to measure photoelectron circular dichroism on chiral molecules, opening the route to table-top time-resolved femtosecond and attosecond chiroptical experiments

International audienceWe photoionize nitrogen molecules with a train of extreme ultraviolet attosecond pulses together with a weak infrared field. We measure the phase of the two-color two-photon ionization transition ͑molecular phase͒ for different states of the ion. We observe a 0.9␲ shift for the electrons produced in the ionization channels leading to the X 2 ⌺ g + , vЈ = 1, and vЈ = 2 states. We relate this phase shift to the presence of a complex resonance in the continuum. By providing both a high spectral and temporal resolution, this general approach gives access to the evolution of extremely short-lived states, which is often not accessible otherwise. DOI: 10.1103/PhysRevA.80.011404 PACS number͑s͒: 33.80.Eh, 33.60.ϩq, 42.65.Ky, 82.53.Kp Ionization of atoms and molecules by absorption of ul-trashort extreme ultraviolet ͑xuv͒ radiation provides rich structural information on the considered species. The ioniza-tion process releases an electron wave packet, which can be described as a coherent superposition of partial waves. The relative contributions and phases of the partial waves can be extracted from photoelectron angular distributions at a given energy ͓1͔. However, the temporal structure of the ejected wave packet, which is imposed by the phase relation between different energy components, is not accessible with such experiments. To access this phase, one needs to couple two energy components of the electron wave packet and record the resulting interference. This can be achieved by absorption of high-order harmonics of an infrared laser pulse in the presence of the fundamental field. An intense laser pulse propagating in a gas jet produces coherent xuv radiation constituted of odd harmonics ͑2q +1͒␻ 0 of the fundamental frequency ␻ 0. These harmonics are all approximately phase locked with the fundamental and form an attosecond pulse train ͑APT͒ ͓2͔. In photoionization experiments with high harmonics, the photoelectron spectrum exhibits equidistant lines resulting from single-photon ionization ͓Fig. 1͑a͔͒. If an additional laser field with frequency ␻ 0 is added, two-photon ionization can occur: absorption of a harmonic photon accompanied by either absorption or stimulated emission of one photon ␻ 0. New lines ͑sidebands͒ appear in the spectrum, in between the harmonics ͓Fig. 1͑a͔͒. Since two coherent quantum paths lead to the same sideband, interferences occur. They are observed in an oscillation of the sideband amplitude as the delay ␶ between the probe ͑ir͒ and harmonic fields is scanned ͓2,3͔. This is the basis of the reconstruction of attosecond beating by interference of two-photon transitions ͑RABBITT͒ technique. The phase of the oscillation is determined by the phase difference between consecutive harmonics ͑phase locking͒ and by additional phase characteristics of the ionization process. The same process can be described in the time domain. The APT creates a train of attosecond electron wave packets. The additional laser field acts as an optical gate on the electrons , which can be used to re...

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High harmonic radiation, produced when intense laser pulses interact with matter, is composed of a train of attosecond pulses. Individual pulses in this train carry information on ultrafast dynamics that vary from one half-optical-cycle to the next. Here, we demonstrate an all-optical photonic streaking measurement that provides direct experimental access to each attosecond pulse by mapping emission time onto propagation angle. This is achieved by inducing an ultrafast rotation of the instantaneous laser wavefront at the focus. We thus time-resolve attosecond pulse train generation, and hence the dynamics in the nonlinear medium itself. We apply photonic streaking to harmonic generation in gases and directly observe, for the first time, the influence of non-adiabatic electron dynamics and plasma formation on the generated attosecond pulse train. These experimental and numerical results also provide the first evidence of the generation of attosecond lighthouses in gases, which constitute ideal sources for attosecond pump-probe spectroscopy.

Optical vortices are currently one of the most intensively studied topics in optics. These light beams, which carry orbital angular momentum (OAM), have been successfully utilized in the visible and infrared in a wide variety of applications. Moving to shorter wavelengths may open up completely new research directions in the areas of optical physics and material characterization. Here, we report on the generation of extreme-ultraviolet optical vortices with femtosecond duration carrying a controllable amount of OAM. From a basic physics viewpoint, our results help to resolve key questions such as the conservation of angular momentum in highly nonlinear light–matter interactions, and the disentanglement and independent control of the intrinsic and extrinsic components of the photon's angular momentum at short-wavelengths. The methods developed here will allow testing some of the recently proposed concepts such as OAM-induced dichroism, magnetic switching in organic molecules and violation of dipolar selection rules in atoms.

Chiral light-matter interactions have been investigated for two centuries, leading to the discovery of many chiroptical processes used for discrimination of enantiomers. Whereas most chiroptical effects result from a response of bound electrons, photoionization can produce much stronger chiral signals that manifest as asymmetries in the angular distribution of the photoelectrons along the light-propagation axis. We implemented self-referenced attosecond photoelectron interferometry to measure the temporal profile of the forward and backward electron wave packets emitted upon photoionization of camphor by circularly polarized laser pulses. We measured a delay between electrons ejected forward and backward, which depends on the ejection angle and reaches 24 attoseconds. The asymmetric temporal shape of electron wave packets emitted through an autoionizing state further reveals the chiral character of strongly correlated electronic dynamics.