Subfemtosecond light pulses can be obtained by superposing several high harmonics of an intense laser pulse. Provided that the harmonics are emitted simultaneously, increasing their number should result in shorter pulses. However, we found that the high harmonics were not synchronized on an attosecond time scale, thus setting a lower limit to the achievable x-ray pulse duration. We showed that the synchronization could be improved considerably by controlling the underlying ultrafast electron dynamics, to provide pulses of 130 attoseconds in duration. We discuss the possibility of achieving even shorter pulses, which would allow us to track fast electron processes in matter.

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

We study photoionization of argon atoms excited by attosecond pulses using an interferometric measurement technique. We measure the difference in time delays between electrons emitted from the 3s(2) and from the 3p(6) shell, at different excitation energies ranging from 32 to 42 eV. The determination of photoemission time delays requires taking into account the measurement process, involving the interaction with a probing infrared field. This contribution can be estimated using a universal formula and is found to account for a substantial fraction of the measured delay.

We study the temporal aspects of laser-assisted extreme ultraviolet (XUV) photoionization using attosecond pulses of harmonic radiation. The aim of this paper is to establish the general form of the phase of the relevant transition amplitudes and to make the connection with the time-delays that have been recently measured in experiments. We find that the overall phase contains two distinct types of contributions: one is expressed in terms of the phase-shifts of the photoelectron continuum wavefunction while the other is linked to continuum-continuum transitions induced by the infrared (IR) laser probe. Our formalism applies to both kinds of measurements reported so far, namely the ones using attosecond pulse trains of XUV harmonics and the others based on the use of isolated attosecond pulses (streaking). The connection between the phases and the time-delays is established with the help of finite difference approximations to the energy derivatives of the phases. The observed time-delay is a sum of two components: a one-photon Wigner-like delay and an universal delay that originates from the probing process itself.

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.

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We present experimental measurements and theoretical calculations of photoionization time delays from the 3s and 3p shells in Ar in the photon energy range of 32-42 eV. The experimental measurements are performed by interferometry using attosecond pulse trains and the infrared laser used for their generation. The theoretical approach includes intershell correlation effects between the 3s and 3p shells within the framework of the random phase approximation with exchange (RPAE). The connection between single-photon ionization and the two-color two-photon ionization process used in the measurement is established using the recently developed asymptotic approximation for the complex transition amplitudes of laser-assisted photoionization. We compare and discuss the theoretical and experimental results especially in the region where strong intershell correlations in the 3s → kp channel lead to an induced "Cooper" minimum in the 3s ionization cross-section.