Study of the spatial and temporal coherence of high order harmonics

We apply the theory of high-order harmonic generation by low-frequency laser fields in the strong field approximation to the study of the spatial and temporal coherence properties of the harmonics. We discuss the role of dynamically induced phases of the atomic polarization in determining the optimal phase matching conditions and angular distributions of harmonics. We demonstrate that the phase matching and the spatial coherence can be controlled by changing the focusing parameters of the fundamental laser beam. Then we present a detailed study of the temporal and spectral properties of harmonics. We discuss how the focusing conditions influence the individual harmonic spectra and time profiles, and how the intensity dependence of the dynamically induced phase leads to a chirp of the harmonic frequency. This phase modulation can be used to control the temporal and spectral properties of the harmonic radiation. Temporally, the harmonic chirped pulse can be recompressed to very small durations. Spectrally, chirping of the fundamental beam may be employed to compensate for the dynamically induced chirp and to control the individual harmonic spectrum. Finally, we discuss the short pulse effects, in particular nonadiabatic phenomena and the possibility of generating attosecond pulses.Comment: Latex file with 37 pages, 25 postscript figures. to appear in Advances in Atomic, Molecular and Optical Physic

Imaging orbitals with attosecond and Ångström resolutions: toward attochemistry? Imaging orbitals with attosecond and Ångström resolutions: toward attochemistry?

International audienceThe recently developed attosecond light sources make the investigation of ultrafast processes in matter possible with unprecedented time resolution. It has been proposed that the very mechanism underlying the attosecond emission allows the imaging of valence orbitals with Ångström space resolution. This controversial idea together with the possibility of combining attosecond and Ångström resolutions in the same measurements has become a hot topic in strong-field science. Indeed , this could provide a new way to image the evolution of the molecular electron cloud during , e. g. a chemical reaction in ' real time '. Here we review both experimental and theoretical challenges raised by the implementation of these prospects. In particular , we show how the valence orbital structure is encoded in the spectral phase of the recombination dipole moment calculated for Coulomb scattering states , which allows a tomographic reconstruction of the orbital using first-order corrections to the plane-wave approach. The possibility of disentangling multi-channel contributions to the attosecond emission is discussed as well as the necessary compromise between the temporal and spatial resolutions. (Some figures may appear in colour only in the online journal

Attosecond emission from chromium plasma

International audienceWe present the first measurement of the attosecond emission generated from underdense plasma produced on a solid target. We generate high-order harmonics of a femtosecond Ti:sapphire laser focused in a weakly ionized underdense chromium plasma. Using the " Reconstruction of Attosecond Beating by Interference of Two-photon Transitions " (RABITT) technique, we show that the 11 th to the 19 th harmonic orders form in the time domain an attosecond pulse train with each pulse having 300 as duration, which is only 1.05 times the theoretical Fourier transform limit. Measurements reveal a very low positive group delay dispersion of 4200 as 2. Beside its fundamental interest, high-order harmonic generation in plasma plumes could thus provide an intense source of attosecond pulses for applications

Spectrally resolved multi-channel contributions to the harmonic emission in N 2

International audienceWhen generated in molecules, high-order harmonics can be emitted through different ionization channels. The coherent and ultrafast electron dynamics occurring in the ion during the generation process is directly imprinted in the harmonic signal, i.e. in its amplitude and spectral phase. In aligned N2 molecules, we find evidence for a fast variation of this phase as a function of the harmonic order when varying the driving laser intensity. Basing our analysis on a three-step model, we find that this phase variation is a signature of transitions from a single- to a multi-channel regime. In particular, we show that significant nuclear dynamics may occur in the ionization channels on the attosecond timescale, affecting both the amplitude and the phase of the harmonic signal

Control of the attosecond synchronization of XUV radiation with phase-optimized mirrors

International audienceWe report on the advanced amplitude and phase control of attosecond radiation allowed by specifically-designed multilayer XUV mirrors. We first demonstrate that such mirrors can compensate for the intrinsic chirp of the attosecond emission over a large bandwidth of more than 20 eV. We then show that their combination with metallic foils introduces a third-order dispersion that is adjustable through the mirror's incidence angle. This results in a controllable beating allowing the radiation to be shaped from a single to a series of sub-100 as pulses

Attosecond chirp-encoded dynamics of light nuclei Attosecond chirp-encoded dynamics of light nuclei

International audienceWe study the spectral phase of high-order harmonic emission as an observable for probing ultrafast nuclear dynamics after the ionization of a molecule. Using a strong-field approximation theory that includes nuclear dynamics, we relate the harmonic phase to the phase of the overlap integral of the nuclear wavefunctions of the initial neutral molecule and the molecular ion after an attosecond probe delay. We determine experimentally the group delay of the high harmonic emission from D 2 and H 2 molecules, which allows us to verify the relation between harmonic frequency and the attosecond delay. The small difference in the harmonic phase between H 2 and D 2 calculated theoretically is consistent with our experimental results

Disentangling Spectral Phases of Interfering Autoionizing States from Attosecond Interferometric Measurements

We have determined spectral phases of Ne autoionizing states from extreme ultraviolet and midinfrared attosecond interferometric measurements and ab initio full-electron time-dependent theoretical calculations in an energy interval where several of these states are coherently populated. The retrieved phases exhibit a complex behavior as a function of photon energy, which is the consequence of the interference between paths involving various resonances. In spite of this complexity, we show that phases for individual resonances can still be obtained from experiment by using an extension of the Fano model of atomic resonances. As simultaneous excitation of several resonances is a common scenario in many-electron systems, the present work paves the way to reconstruct electron wave packets coherently generated by attosecond pulses in systems larger than heliumWork supported by the ERC proof-of-concept Grant No. 780284-Imaging-XChem within the seventh framework program of the European Union, the MINECO Project No. FIS2013-42002-R, the EU-H2020- LASERLABEUROPE-654148, the ANR Projects No. ANR-15-CE30-0001-CIMBAAD, No. ANR-11- EQPX0005-ATTOLAB, and No. ANR-10-LABX-0039- PALM, the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award no. DEGF02-04ER15614, and the NSF Grant No. PHY-1607588. Calculations were performed at CCC-UAM and Marenostrum Supercomputer Center. F. M. acknowledges support from the “Severo Ochoa” Programme for Centres of Excellence in R&D (MINECO, Grant No. SEV-2016- 0686) and the “María de Maeztu” Programme for Units of Excellence in R&D (Grant No. MDM-2014-0377

Amplitude and phase control of attosecond light pulses

We report the generation, compression, and delivery on target of ultrashort extreme-ultraviolet light pulses using external amplitude and phase control. Broadband harmonic radiation is first generated by focusing an infrared laser with a carefully chosen intensity into a gas cell containing argon atoms. The emitted light then goes through a hard aperture and a thin aluminum filter that selects a 30-eV bandwidth around a 30-eV photon energy and synchronizes all of the components, thereby enabling the formation of a train of almost Fourier-transform-limited single-cycle 170 attosecond pulses. Our experiment demonstrates a practical method for synthesizing and controlling attosecond waveforms. © 2005 The American Physical Society