Α 10-gigawatt attosecond source for non-linear XUV optics and XUV-pump-XUV-probe studies.

The quantum mechanical motion of electrons and nuclei in systems spatially confined to the molecular dimensions occurs on the sub-femtosecond to the femtosecond timescales respectively. Consequently, the study of ultrafast electronic and, in specific cases, nuclear dynamics requires the availability of light pulses with attosecond (asec) duration and of sufficient intensity to induce two-photon processes, essential for probing the intrinsic system dynamics. The majority of atoms, molecules and solids absorb in the extreme-ultraviolet (XUV) spectral region, in which the synthesis of the required attosecond pulses is feasible. Therefore, the XUV spectral region optimally serves the study of such ultrafast phenomena. Here, we present a detailed review of the first 10-GW class XUV attosecond source based on laser driven high harmonic generation in rare gases. The pulse energy of this source largely exceeds other laser driven attosecond sources and is comparable to the pulse energy of femtosecond Free-Electron-Laser (FEL) XUV sources. The measured pulse duration in the attosecond pulse train is 650 ± 80 asec. The uniqueness of the combined high intensity and short pulse duration of the source is evidenced in non-linear XUV-optics experiments. It further advances the implementation of XUV-pump-XUV-probe experiments and enables the investigation of strong field effects in the XUV spectral region.

Next Generation Driver for Attosecond and Laser-plasma Physics.

The observation and manipulation of electron dynamics in matter call for attosecond light pulses, routinely available from high-order harmonic generation driven by few-femtosecond lasers. However, the energy limitation of these lasers supports only weak sources and correspondingly linear attosecond studies. Here we report on an optical parametric synthesizer designed for nonlinear attosecond optics and relativistic laser-plasma physics. This synthesizer uniquely combines ultra-relativistic focused intensities of about 1020 W/cm2 with a pulse duration of sub-two carrier-wave cycles. The coherent combination of two sequentially amplified and complementary spectral ranges yields sub-5-fs pulses with multi-TW peak power. The application of this source allows the generation of a broad spectral continuum at 100-eV photon energy in gases as well as high-order harmonics in relativistic plasmas. Unprecedented spatio-temporal confinement of light now permits the investigation of electric-field-driven electron phenomena in the relativistic regime and ultimately the rise of next-generation intense isolated attosecond sources.

Polarization shaping of high-order harmonics in laser-aligned molecules.

The present work reports on the generation of short-pulse coherent extreme ultraviolet radiation of controlled polarization. The proposed strategy is based on high-order harmonics generated in pre-aligned molecules. Field-free molecular alignment produced by a short linearly-polarized infrared laser pulse is used to break the isotropy of a gas medium. Driving the aligned molecules by a circularly-polarized infrared pulse allows to transfer the anisotropy of the medium to the polarization of the generated harmonic light. The ellipticity of the latter is controlled by adjusting the angular distribution of the molecules at the time they interact with the driving pulse. Extreme ultraviolet radiation produced with high degree of ellipticity (close to circular) is demonstrated.

The ion microscope as a tool for quantitative measurements in the extreme ultraviolet.

We demonstrate a tool for quantitative measurements in the extreme ultraviolet (EUV) spectral region measuring spatially resolved atomic ionization products at the focus of an EUV beam. The ionizing radiation is a comb of the 11(th)-15(th) harmonics of a Ti:Sapphire femtosecond laser beam produced in a Xenon gas jet. The spatial ion distribution at the focus of the harmonics is recorded using an ion microscope. Spatially resolved single- and two-photon ionization products of Argon and Helium are observed. From such ion distributions single- and two-photon generalized cross sections can be extracted by a self-calibrating method. The observation of spatially resolved two-EUV-photon ionization constitutes an initial step towards future single-shot temporal characterization of attosecond pulses.

A compact collinear polarization gating scheme for many cycle laser pulses.

We demonstrate the generation of a broadband coherent continuum extreme-ultraviolet (XUV) radiation produced by the interaction of gases with a many-cycle infrared (IR) laser field, utilizing a compact collinear many cycle-polarization gating (CMC-PG) device. The spectral width of the XUV radiation can support isolated pulses of 200 asec duration. The CMC-PG device forms a high energy content ultra-short temporal gate in a many-cycle laser pulse, within which the XUV emission is taking place. The gate width has been measured and is in agreement with the theoretical calculations. The simplicity, the compactness, the long term stability, and the high IR energy output within the gate, make the CMC-PG device an ideal tool for generating energetic isolated attosecond pulses and measure the carrier-envelope phase of a high-power many-cycle laser field.

Tracking autoionizing-wave-packet dynamics at the 1-fs temporal scale.

We present time-resolved studies and Fourier transform spectroscopy of inner-shell excited states undergoing Auger decay and doubly excited autoionizing states, utilizing coherent extreme-ultraviolet (XUV) radiation continua. Series of states spanning a range of ∼4 eV are excited simultaneously. An XUV probe pulse tracks the oscillatory and decaying evolution of the formed wave packet. The Fourier transform of the measured trace reproduces the spectrum of the series. The present work paves the way for ultrabroadband XUV spectroscopy and studies of ultrafast dynamics in all states of matter.

Coherent continuum extreme ultraviolet radiation in the sub-100-nJ range generated by a high-power many-cycle laser field.

High-energy coherent continuum radiation is generated by the interaction of rare gases with a high-power many-cycle laser field, utilizing the interferometric polarization gating technique. A narrow temporal gate is formed in the laser pulse within which the extreme ultraviolet (XUV) emission is restricted. An analytical expression for the gate function is derived. A super-XUV continuum down to 15 nm, broad enough to support synthesis of single pulses of 260 as duration and a few tens of nanojoule energy, has been measured. These results directly challenge the perspectives of single-attosecond pulse XUV-pump-XUV-probe applications.

Spectral phase distribution retrieval through coherent control of harmonic generation.

The temporal intensity distribution of the third harmonic of a Ti:sapphire laser generated in Xe gas is fully reconstructed from its spectral phase and amplitude distributions. The spectral phases are retrieved by cross correlating the fundamental laser frequency field with that of the third harmonic, in a three laser versus one harmonic photon coupling scheme. The third harmonic spectral amplitude distribution is extracted from its field autocorrelation. The measured pulse duration is found to be in agreement with that expected from lowest order perturbation theory both for unstretched and chirped pulses.

Second order autocorrelation of an XUV attosecond pulse train.

Temporal widths of an attosecond (asec) XUV radiation pulse train, formed by the superposition of higher order harmonics, have been recently determined utilizing a 2nd order autocorrelation measurement. An assessment of the validity of the approach, for the broadband XUV radiation of asec pulses, is implemented through ab initio calculations modeling the spectral and temporal response of the two-XUV-photon He ionization detector employed. The measured width of the asec bursts is discussed in terms of the spectral phases of the individual harmonics, as well as in terms of the spatially modulated temporal width of the radiation, and is found in reasonable agreement with the expected duration.

Direct observation of attosecond light bunching.

Temporal probing of a number of fundamental dynamical processes requires intense pulses at femtosecond or even attosecond (1 as = 10(-18) s) timescales. A frequency 'comb' of extreme-ultraviolet odd harmonics can easily be generated in the interaction of subpicosecond laser pulses with rare gases: if the spectral components within this comb possess an appropriate phase relationship to one another, their Fourier synthesis results in an attosecond pulse train. Laser pulses spanning many optical cycles have been used for the production of such light bunching, but in the limit of few-cycle pulses the same process produces isolated attosecond bursts. If these bursts are intense enough to induce a nonlinear process in a target system, they can be used for subfemtosecond pump-probe studies of ultrafast processes. To date, all methods for the quantitative investigation of attosecond light localization and ultrafast dynamics rely on modelling of the cross-correlation process between the extreme-ultraviolet pulses and the fundamental laser field used in their generation. Here we report the direct determination of the temporal characteristics of pulses in the subfemtosecond regime, by measuring the second-order autocorrelation trace of a train of attosecond pulses. The method exhibits distinct capabilities for the characterization and utilization of attosecond pulses for a host of applications in attoscience.

Two-Photon Ionization of He through a Superposition of Higher Harmonics.

We present experimental results and theoretical analysis of two-photon ionization of He by a superposition of the 7th to the 13th harmonic of a Ti:sapphire laser. Solving the time-dependent Schrödinger equation for He in a coherent polychromatic field, the He+ yield is calculated. From this yield the number of He+ ions produced has been estimated and found in reasonable agreement with its measured value. The present results establish the feasibility of a second-order autocorrelation measurement of superposition of harmonics, and thus they represent the precursor towards the direct temporal characterization of attosecond pulse trains.

Temporal characterization of short-pulse third-harmonic generation in an atomic gas by a transmission-grating Michelson interferometer.

By use of a transmission-grating-based Michelson interferometer, second-order interferometric as well as intensity autocorrelation traces of the third harmonic of a Ti:sapphire 50-fs laser beam produced in Ar have been measured. The duration of the harmonic is found to be that expected from lowest-order perturbation theory. At this wavelength, the performance of the interferometer with respect to pulse-front distortion and dispersion is found to be satisfactory. This result is a first step toward the use of the interferometer for the temporal characterization of higher harmonics or harmonic superposition forming attosecond pulse trains.

Charge-state resolved above threshold ionization

Photoelectron energy resolved spectra recorded in coincidence with singly and doubly ionized atoms are reported for the interaction of xenon with 60 fs laser pulses at 800 nm and 1x10(14) W/cm(2). Double ionization contributions in the spectrum have been established. The appearance of a single ionization plateau in above threshold ionization is verified. A hotter electron distribution is found for the double ionization.