Macroscopic effects in attosecond pulse generation

We examine how the generation and propagation of high-order harmonics in a partly ionized gas medium affect their strength and synchronization. The temporal properties of the resulting attosecond pulses generated in long gas targets can be significantly influenced by macroscopic effects, in particular by the intensity in the medium and the degree of ionization. Under some conditions, the use of gas targets longer than the absorption length can lead to the generation of self-compressed attosecond pulses. We show this effect experimentally, using long argon-filled gas cells as generating medium.Comment: 5 pages 4 figure

Theory of attosecond delays in laser-assisted photoionization

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. This makes clear that the observed time-delays is a sum of two components: a one-photon Wigner-like delay and an universal delay that originates from the probing process itself.Comment: 15 pages, 10 figures, special issue 'Attosecond spectroscopy' Chem. Phy

Phase Measurement of Resonant Two-Photon Ionization in Helium

We study resonant two-color two-photon ionization of Helium via the 1s3p 1P1 state. The first color is the 15th harmonic of a tunable titanium sapphire laser, while the second color is the fundamental laser radiation. Our method uses phase-locked high-order harmonics to determine the {\it phase} of the two-photon process by interferometry. The measurement of the two-photon ionization phase variation as a function of detuning from the resonance and intensity of the dressing field allows us to determine the intensity dependence of the transition energy.Comment: 4 pages, 5 figures, under consideratio

High-order Harmonic Generation and Dynamic Localization in a driven two-level system, a non-perturbative solution using the Floquet-Green formalism

We apply the Floquet-Green operator formalism to the case of a harmonically-driven two-level system. We derive exact expressions for the quasi-energies and the components of the Floquet eigenstates with the use of continued fractions. We study the avoided crossings structure of the quasi-energies as a function of the strength of the driving field and give an interpretation in terms of resonant multi-photon processes. From the Floquet eigenstates we obtain the time-evolution operator. Using this operator we study Dynamic Localization and High-order Harmonic Generation in the non-perturbative regime

Angular distributions of high-order harmonics generated by a femtosecond laser

We present a systematic study of the angular distributions of high-order harmonics generated with a femtosecond Cr:LiSrAlF6 laser. We investigate the influence of different parameters, namely laser intensity, nonlinear order, nature of the gas and position of the laser focus relative to the generating medium. We show that when the laser is focused before the atomic medium, harmonics with regular spatial profiles can be generated with reasonable conversion efficiency. Their divergence does not depend directly on the nonlinear order, the intensity or even the nature of the generating gas, but rather on the region of the spectrum the considered harmonic belongs to, which is determined by the combination of the three preceding elements. When the focus is drawn closer to the medium, the distributions get increasingly distorted, becoming annular with a significant divergence for a focus right into-or after-the jet. We perform numerical simulations of the angular distributions. The simulated profiles reproduce remarkably well the experimental trends and are thus used to interpret them

Probing single-photon ionization on the attosecond time scale

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 single photoemission time delays requires to take into account the measurement process, involving the interaction with a probing infrared field. This contribution can be estimated using an universal formula and is found to account for a substantial fraction of the measured delay.Comment: 4 pages, 4 figures, under consideratio

Photoionization in the time and frequency domain

Ultrafast processes in matter, such as the electron emission following light absorption, can now be studied using ultrashort light pulses of attosecond duration ($10^{-18}$s) in the extreme ultraviolet spectral range. The lack of spectral resolution due to the use of short light pulses may raise serious issues in the interpretation of the experimental results and the comparison with detailed theoretical calculations. Here, we determine photoionization time delays in neon atoms over a 40 eV energy range with an interferometric technique combining high temporal and spectral resolution. We spectrally disentangle direct ionization from ionization with shake up, where a second electron is left in an excited state, thus obtaining excellent agreement with theoretical calculations and thereby solving a puzzle raised by seven-year-old measurements. Our experimental approach does not have conceptual limits, allowing us to foresee, with the help of upcoming laser technology, ultra-high resolution time-frequency studies from the visible to the x-ray range.Comment: 5 pages, 4 figure