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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.

Intense laser-matter interactions are at the center of interest in research and technology since the development of high power lasers. They have been widely used for fundamental studies in atomic, molecular, and optical physics, and they are at the core of attosecond physics and ultrafast opto-electronics. Although the majority of these studies have been successfully described using classical electromagnetic fields, recent investigations based on fully quantized approaches have shown that intense laser-atom interactions can be used for the generation of controllable high-photon-number entangled coherent states and coherent state superpositions. In this tutorial, we provide a comprehensive fully quantized description of intense laser-atom interactions. We elaborate on the processes of high harmonic generation, above-threshold-ionization, and we discuss new phenomena that cannot be revealed within the context of semi-classical theories. We provide the description for conditioning the light field on different electronic processes, and their consequences for quantum state engineering of light. Finally, we discuss the extension of the approach to more complex materials, and the impact to quantum technologies for a new photonic platform composed by the symbiosis of attosecond physics and quantum information science., Comment: 43 pages, 19 figures, Tutorial including new results

We present the results of microscopic and macroscopic simulations on electron quantum path interferences during high harmonic generation in atomic gas medium driven by various ultrashort chirped driving laser pulses.

In the present work we report on the current progress of the recently constructed GW attosecond extreme ultraviolet (XUV) source developed at the Institute of Electronic Structure and Laser of the Foundation for Research and Technology-Hellas (I.E.S.L-FO.R.T.H.). By the implementation of a compact-collinear polarization gating arrangement, the generation of a broadband, coherent XUV quasi-continuum produced by the interaction of a many-cycle infrared field with a gas phase medium is achieved. The spectral width of the XUV emission generated in Xenon, is spanning in the range of 17-32 eV and can support isolated pulses of duration in the range from 0.4 fs to 1.3 fs and pulse energy in the 1 {\mu}J level.Theoretical calculations, taking into account the experimental conditions of this work, are supporting the observations, offering also an insight regarding the temporal profile of the emitted radiation. Finally, the high intensity of the produced XUV pulses has been confirmed by investigating the two-XUV-photon double ionization process of Argon atoms. The demonstrated results inaugurate the capability of the beamline to produce intense isolated attosecond pulses towards their exploitation in studies of non-linear XUV processes, attosecond pulse metrology and XUV pump XUV probe experiments., Comment: 18 pages, 6 figures

We present a theoretical demonstration on the generation of entangled coherent states and of coherent state superpositions, with photon numbers and frequencies orders of magnitude higher than those provided by the current technology. This is achieved by utilizing a quantum mechanical multimode description of the single- and two-color intense laser field driven process of high harmonic generation in atoms. It is found that all field modes involved in the high harmonic generation process are entangled, and upon performing a quantum operation, leads to the generation of high photon number optical cat states spanning from the far infrared to the extreme-ultraviolet spectral region. This provides direct insights into the quantum mechanical properties of the optical field in intense laser matter interaction. Finally, these states can be considered as a new resource for fundamental tests of quantum theory, quantum information processing or sensing with non-classical states of light., 5 pages (3 figures) + 4 pages supplement (2 figures)

Attoscience is the emerging field that accesses the fastest electronic processes occurring at the atomic and molecular length scales with attosecond (1 as = 1 0 − 18 s) time resolution having wide ranging physical, chemical, material science and biological applications. The quintessential and one of the most fundamental processes in this domain is the generation of phase locked XUV attosecond pulses. The theoretical approach to understand the process incorporates a fully quantum or semi classical or relativistic description of coherent charge dynamics in intense ultrashort electromagnetic fields driving a quantum system (an atom, a molecule, solid band gap materials or surface plasmas). Modelling of such physical and dynamical systems in science and also in many other branches often leads to equations represented in terms of complex multi-dimensional integrals. These integrals can often be solved using the stationary phase approximation, which leads to a series of equations identifying the points in the multi-dimensional space, having most significant contributions in their evaluation. These points are usually indicated as saddle points. The description of the dynamics of quantum mechanical or relativistic systems that results from such an approach enables near to classical physics intuitive perceptions of the processes under investigation. Thus, the saddle point methods are very powerful and valuable general theoretical tools to obtain asymptotic expressions of such solutions and help also to gain physical insights on the underlying phenomena. Such techniques developed in the past have been adapted to study the emission of as pulses by different physical systems and have been widely employed in calculating and estimating the response of matter to intense electromagnetic pulses on ultrafast time scales. Here we provide an extensive disposition of the saddle point approaches unifying their ubiquitous applications within the domain of attoscience valid for simple atomic to more complex condensed matter systems undergoing ultrafast dynamics and present current trends and advancements in the field. In this review we would delineate the methodology, present a synthesis of seminal works and describe the state of the art applications. Finally we also address ultrashort time dynamics of novel materials that have gained much attention recently, namely lower dimensional material systems and micro-plasma systems.

International audience; Quantum-optical spectrometry is a recently developed shot-to-shot photon correlation-based method, namely using a quantum spectrometer (QS), that has been used to reveal the quantum optical nature of intense laser–matter interactions and connect the research domains of quantum optics (QO) and strong laser-field physics (SLFP). The method provides the probability of absorbing photons from a driving laser field towards the generation of a strong laser–field interaction product, such as high-order harmonics. In this case, the harmonic spectrum is reflected in the photon number distribution of the infrared (IR) driving field after its interaction with the high harmonic generation medium. The method was implemented in non-relativistic interactions using high harmonics produced by the interaction of strong laser pulses with atoms and semiconductors. Very recently, it was used for the generation of non-classical light states in intense laser–atom interaction, building the basis for studies of quantum electrodynamics in strong laser-field physics and the development of a new class of non-classical light sources for applications in quantum technology. Here, after a brief introduction of the QS method, we will discuss how the QS can be applied in relativistic laser–plasma interactions and become the driving factor for initiating investigations on relativistic quantum electrodynamics.

Recently, using conditioning approaches on the high-harmonic generation process induced by intense laser-atom interactions, we have developed a new method for the generation of optical Schrodinger cat states (Lewenstein et al. in Nat Phys, 17 1104–1108, 2021. https://doi/10.1038/s41567-021-01317-w). These quantum optical states have been proven to be very manageable as, by modifying the conditions under which harmonics are generated, one can interplay between kitten and genuine cat states. Here, we demonstrate that this method can also be used for the development of new schemes towards the creation of optical Schrodinger cat states, consisting of the superposition of three distinct coherent states. Apart from the interest these kind of states have on their own, we additionally propose a scheme for using them towards the generation of large cat states involving the sum of two different coherent states. The quantum properties of the obtained superpositions aim to significantly increase the applicability of optical Schrodinger cat states for quantum technology and quantum information processing.

High-harmonic generation (HHG) in crystals offers a simple, affordable and easily accessible route to carrier-envelope phase (CEP) measurements, which scales favorably towards longer wavelengths. We present measurements of HHG in ZnO using few-cycle pulses at 3.1µm. Thanks to the broad bandwidth of the driving laser pulses, spectral overlap between adjacent harmonic orders is achieved. The resulting spectral interference pattern provides access to the relative harmonic phase, and hence, the CEP.

Electron quantum path interferences in strongly laser-driven aligned molecules and their dependence on the molecular alignment is an essential open problem in strong-field molecular physics. Here, we demonstrate an approach which provides direct access to the observation of these interference processes. The approach is based on the combination of the time-gated-ion-microscopy technique with a pump-probe arrangement used to align the molecules and generate high-order harmonics. By spatially resolving the interference pattern produced by the spatiotemporal overlap of the harmonics emitted by the short and long electron quantum paths, we have succeeded in measuring in situ their phase difference and disclose their dependence on molecular alignment. The findings constitute a vital step towards an understanding of strong-field molecular physics and the development of attosecond spectroscopy approaches without the use of auxiliary atomic references., Comment: 7 pages, 3 figures

Motivated by the achieved high intensities of novel extreme ultraviolet (XUV) radiation sources, such as free electron lasers and laser-driven high harmonic generation beamlines, we elaborate on their perspective in inducing observable strong field effects. The feasibility of extending such effects from the infrared and visible spectral regimes in the XUV domain is supported through numerically calculated models of near-future experiments. We highlight the advancement of performing studies in the time domain, using ultra-short XUV pulses, which allows for the temporal evolution of such effects to be followed. Experimental and theoretical obstacles and limitations are further discussed. © The Author(s), 2020. Published by Cambridge University Press in association with Chinese Laser Press.

The long-standing scientific quest of real-time tracing electronic motion and dynamics in all states of matter has been remarkably benefited by the development of intense laser-based pulsed sources with a temporal resolution in the attosecond [1 attosecond = 10−18 s] time scale. Nowadays, attosecond pulses are routinely produced in laboratories by the synthesis of the frequency components of broadband coherent extreme ultraviolet (XUV) radiation generated by the interaction of matter with intense femtosecond (fs) pulses. Attosecond pulse metrology aims at the accurate and complete determination of the temporal and phase characteristics of attosecond pulses and is one of the most innovative challenges in the broad field of ultrashort pulse metrology. For more than two decades since coherent high-brilliance broadband XUV sources have become available, fascinating advances in attosecond pulse metrology have led to the development of remarkable techniques for pulse duration measurements as well as the complete reconstruction of those pulses. Nonetheless, new challenges born from diverse fields call upon for additional efforts and continuously innovative ideas in the field. In this perspective article, we follow the history of ultrashort pulse technology tracing attosecond pulse production and characterization approaches, focus on the operation principles of the most commonly used techniques in the region where they interact with matter, address their limitations, and discuss future prospects as well as endeavors of the field to encounter contemporary scientific progress.

Electrodynamical processes induced in complex systems like semiconductors by strong electromagnetic fields have traditionally been described using semiclassical approaches. Although these approaches allowed the investigation of ultrafast dynamics in solids culminating in multipetahertz electronics, they do not provide any access to the quantum-optical nature of the interaction, as they treat the driving field classically and unaffected by the interaction. Here, using a full quantum-optical approach, we demonstrate that the subcycle electronic response in a strongly driven semiconductor crystal is imprinted in the quantum state of the driving field resulting in nonclassical light states carrying the information of the interaction. This vital step towards strong-field ultrafast quantum electrodynamics unravels information inaccessible by conventional approaches and leads to the development of a new class of nonclassical light sources.

We report the application of the time gated ion microscopy technique in accessing online the position of the source of harmonics generated in atomic gas media. This is achieved by mapping the spatial extreme-ultraviolet (XUV)-intensity distribution of the harmonic source onto a spatial ion distribution, produced in a separate focal volume of the generated XUV beam through single photon ionization of atoms. It is found that the position of the harmonic source depends on the relative position of the harmonic generation gas medium and the focus of the driving infrared (IR) beam. In particular, by translating the gas medium with respect to the IR beam focus different virtual source positions are obtained online. Access to such online source positioning allows better control and provides increased possibilities in experiments where selection of electron trajectory is important. The present study gives also access to quantitative information which is connected to the divergence, the coherence properties and the photon flux of the harmonics. Finally, it constitutes a precise direct method for providing complementary experimental info to different attosecond metrology techniques., Comment: 7 pages, 3 figures

Relativistic surface high harmonics have been considered a unique source for the generation of intense isolated attosecond pulses in the extreme ultra-violet and x-ray spectral ranges. Their practical realization, however, is still a challenging task and requires identification of optimum experimental conditions and parameters. Here, we present measurements and particle-in-cell simulations to determine the optimum values for the most important parameters. In particular, we investigate the dependence of harmonics efficiency, divergence, and beam quality on the pre-plasma scale length as well as identify the optimum conditions for generation of isolated attosecond pulses by measuring the dependence of the harmonics spectrum on the carrier - envelope phase of the driving infrared field. (C) 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

The interpretation of experimental data from novel mid-infrared few-cycle laser sources requires an understanding of ionization mechanisms and knowledge about related ion yields. Experimental studies have indicated sequential double ionization as the dominant process above 1014 W cm−2. These results contradict a recent prediction that in this spectral region, non-sequential processes dominate the double ionization of xenon up to intensities of about 1015 W cm−2. In either case, the ratio of doubly to singly charged xenon yield reported in previous studies has been limited to a few percent, indicating a regime well below the onset of saturation of the double ionization process. We present an experimental study of double ionization of xenon and krypton atoms exposed to intense near four-cycle pulses at 3.2 μm. Our experiments rely on the ion microscopy technique, which facilitates the detection of ions originating from a restricted region within the interaction volume, thereby reducing the impact of focal averaging. Our measurements suggest that at intensities of close to 1.2 × 1014 W cm−2, double ionization of xenon and krypton is already significantly saturated. In particular, we find a doubly to singly charged yield ratio of about 75 percent for xenon and 25 percent for krypton. We compare our results with the predictions of different models accounting for the effects of volume averaging and focal geometry. We find that in the deeply saturated regime of our experiment, the Perelomov–Popov–Terentyev theory significantly underestimates the observed double ionization yield.

Along with the review of the technological frame that will be available at the Extreme Light Infrastructure Attosecond Light Pulse Source (ELI-ALPS) we present considerations applicable to large-scale attosecond sources driven by high-power laser pulses.

We demonstrate multiphoton ionization of inner-shell electrons in Xenon with 100-eV attosecond pulses. This was achieved with a novel XUV source based on high-harmonic generation in the gas phase driven with multi-TW few-cycle laser pulses.

Nonlinear light-matter interactions in the extreme ultraviolet (XUV) are a prerequisite to perform XUV-pump/XUV-probe spectroscopy of core electrons. Such interactions are now routinely investigate ...

Ultrashort extreme ultraviolet (EUV) laser pulses with a controllable polarization state are highly desirable for time-resolved studies and applications involving chirality, circular dichroism, spin dynamics and magnetism in the gas phase or condensed matter. A convenient method to generate such radiation is higher-order harmonic generation (HHG) as applied in numerous laboratories worldwide. Unless special techniques are employed, however, this process will produce predominantly linearly polarized EUV radiation as imposed by the symmetry of the generating field-medium system. To overcome this fundamental limitation, intense research activity has focused on shaping the time-dependent field vector of the generating light pulse [1]. In the current contribution we present an alternative method to generate EUV pulses with a widely controllable polarization state utilizing field-free aligned molecules as an anisotropically shaped medium for HHG.

High-order harmonics in the extreme-ultraviolet spectral range, resulting from the strong-field laser-atom interaction, have been used in a broad range of fascinating applications in all states of matter. In the majority of these studies the harmonic generation process is described using semi-classical theories which treat the electromagnetic field of the driving laser pulse classically without taking into account its quantum nature. In addition, for the measurement of the generated harmonics, all the experiments require diagnostics in the extreme-ultraviolet spectral region. Here by treating the driving laser field quantum mechanically we reveal the quantum-optical nature of the high-order harmonic generation process by measuring the photon number distribution of the infrared light exiting the harmonic generation medium. It is found that the high-order harmonics are imprinted in the photon number distribution of the infrared light and can be recorded without the need of a spectrometer in the extreme-ultraviolet., Describing the properties of high harmonic photons is challenging due to the complexity of XUV spectroscopy. Here the authors use the photon statistics of the transmitted infrared laser photons to characterize the XUV photon flux without the need of XUV spectrometers.

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.

Studies of ultrafast dynamics along with femtosecond-pulse metrology rely on non-linear processes, induced solely by the exciting/probing pulses or the pulses to be characterized. Extension of these approaches to the extreme-ultraviolet (XUV) spectral region opens up a new, direct route to attosecond scale dynamics. Limitations in available intensities of coherent XUV continua kept this prospect barren. The present work overcomes this barrier. Reaching condition at which simultaneous ejection of two bound electrons by two-XUV-photon absorption becomes more efficient than their one-by-one removal it is succeeded to probe atomic coherences, evolving at the 1fs scale, and determine the XUV-pulse duration. The investigated rich and dense in structure autoionizing manifold ascertains applicability of the approach to complex systems. This initiates the era of XUV-pump-XUV-probe experiments with attosecond resolution., 27 pages

The population dynamics induced in an atomic system by XUV-attosecond radiation have been investigated within the electric dipole approximation. The main characteristics of the dynamics are explained in simple terms, extending our previous work on coherent laser-atom interactions in the XUV spectral region. Attosecond beating appearing in a second-order autocorrelation of a coherent superposition of high order harmonics, is investigated from the perspective of a superposition of Rabi oscillations, as well as of coherent population return (CPR). The work reveals the strength of attosecond radiation as a tool for time domain studies of coherent manipulations of quantum systems.

An experiment demonstrating the generation of subfemtosecond pulses of light through the interaction of laser light with a solid target underlines the potential of this approach to lead to a new generation of intense sources of attosecond pulses.

Continuing efforts in ultrashort pulse engineering have recently led to the breakthroughs of the generation of attosecond (10−18 s) pulse trains1,2,3,4,5,6,7 and isolated pulses8,9,10,11. Although trains of multiple pulses can be generated through the interaction of many-optical-cycle pulses with gases—a process that has led to intense extreme-ultraviolet emission3,4,5—the generation of isolated high-intensity pulses, which requires few-cycle driving pulses, remains a challenge. Here, we report a vital step towards the generation of such pulses, the production of broad continuum extreme-ultraviolet emission using a high-intensity, many-cycle, infrared pulsed laser, through the interferometric modulation of the ellipticity of 50-fs-long driving pulses. The increasing availability of high-power many-cycle lasers and their potential use in the construction of intense attosecond radiation—with either gas or solid-surface targets12—offer exciting opportunities for multiphoton extreme-ultraviolet-pump–extreme-ultraviolet-probe studies of laser–matter and laser–plasma interactions.

We present the theory and experimental details for chiral-cavity-ring-down polarimetry and magnetometry, based on ring cavities supporting counterpropagating laser beams. The optical-rotation symmetry is broken by the presence of both chiral and Faraday birefringence, giving rise to signal reversals which allow rapid background subtractions. We present the measurement of the specific rotation at 800 nm of vapors of α-pinene, 2-butanol, and α-phellandrene, the measurement of optical rotation of sucrose solutions in a flow cell, the measurement of the Verdet constant of fused silica, and measurements and theoretical treatment of evanescent-wave optical rotation at a prism surface. Therefore, these signal-enhancing and signal-reversing methods open the way for ultrasensitive polarimetry measurements in gases, liquids and solids, and at surfaces.

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 11th–15th 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.

Recent developments in the generation, metrology and potential applications of XUV-attosecond (as) pulses, formed by the coherent superposition of harmonics of an infrared femtosecond (fs) laser pulse, are reviewed. Particular emphasis is given to the recently achieved second-order autocorrelation (AC) measurement of a sub-femtosecond (sub-fs) pulse train. The method is a non-trivial extension in the XUV spectral range of the well-established technique routinely used in ‘fs’ pulse metrology. Besides the direct visualization of a periodic attosecond structure and the quantitative information it supplies, the approach introduces a unique technique for the implementation of XUV-pump XUV-probe type of experimental studies of ultra-fast phenomena. It further relates to the metrology and time domain application interests of other advanced XUV radiation sources, such as the XFEL-based installations. While the implementation of the method and its refined versions with laser harmonics is a challenge at the limits of the realizable, the profoundly high scheduled intensities of XFEL sources are expected to sufficiently enhance its robustness and range of applicability.

The unequivocal demonstration of attosecond XUV pulse train generation based on the synthesis of a comb of harmonics of an infrared femtosecond laser pulse is inevitably linked to a reliable method of pulse characterization in this temporal regime. The most commonly used method to date relies on a cross-correlation technique between the fundamental laser frequency and the XUV light from which a measurement of the relative phases of the consecutive harmonics is obtained and the attosecond temporal structure in a train of XUV pulses is inferred. Here we report on an alternative method that renders possible the direct observation of a train of attosecond pulses in form of a second-order autocorrelation trace. The method is an extension in the XUV spectral range of the well-established technique commonly used for the characterization of femtosecond laser pulses. Besides being the first direct visualization of a periodic attosecond structure, the approach supplies quantitative information on the overall pulse ...

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 train1,2. Laser pulses spanning many optical cycles have been used for the production of such light bunching3,4, but in the limit of few-cycle pulses the same process produces isolated attosecond bursts5,6. If these bursts are intense enough to induce a nonlinear process in a target system7,8,9, they can be used for subfemtosecond pump–probe studies of ultrafast processes. To date, all methods for the quantitative investigation of attosecond light localization4,6,10 and ultrafast dynamics11 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.

Journal of physics / B 50(13), 132002 - (2017). doi:10.1088/1361-6455/aa6ee8, This review presents the technological infrastructure that will be available at the Extreme Light Infrastructure Attosecond Light Pulse Source (ELI-ALPS) international facility. ELI-ALPS will offer to the international scientific community ultrashort pulses in the femtosecond and attosecond domain for time-resolved investigations with unprecedented levels of high quality characteristics. The laser sources and the attosecond beamlines available at the facility will make attosecond technology accessible for scientists lacking access to these novel tools. Time-resolved investigation of systems of increasing complexity is envisaged using the end stations that will be provided at the facility., Published by IOP Publ., Bristol

Through frequency up-conversion of polarization-shaped, femtosecond laser pulses nonlinearly interacting with xenon atoms, energetic, broadband, coherent, XUV continuum radiation is generated. By exploiting the thus-formed short-duration XUV pulses, all the optically allowed excited states of H2 are coherently populated. Nuclear and electronic 1-fs-scale dynamics are subsequently investigated by means of XUV-pump-XUV-probe measurements, which are compared to the results of ab initio calculations. The revealed dynamics reflects the intrinsic molecular behavior, as the XUV probe pulse hardly distorts the molecular potential, This work is supported in part by the European Commission programs ATTOFEL, CRISP, Laserlab Europe, the European COST Actions MPI1203-SKO and CM1204 XLIC, and the Greek funding program NSRF. A.P. and F.M. acknowledge allocation of computer time by CCC-UAM and BSC Mare Nostrum, and financial support from the Advanced Grant of the European Research Council XCHEM (No. 290853), the European grant MC-RG ATTOTREND, the MICINN Project (No. FIS2010-15127), and the ERA-Chemistry Project (No. PIM2010EEC-00751).

Intense isolated attosecond pulses with >100 eV photon energy are produced via high-order-harmonic generation using 80mJ sub-5 fs laser pulses. The generation of these attosecond pulses and their application to non-linear XUV-XUV pum-probe experiments is discussed.

Exploiting intense coherent XUV continua, supporting attosecond pulse formation, we have performed the first ever XUV-pump-XUV-probe studies of 1fs scale dynamics in atoms and molecules. Progress towards single shot non-linear XUV autocorrelation is also reported.

The tunnelling of an electron through a suppressed atomic potential followed by its motion in the continuum, is the fundamental mechanism underlying strong-field laser-atom/molecule interactions. Due to its quantum nature, the interaction is governed by the phase of the released electron wave-packets. Thus, detailed mapping of the electron wave-packet interferences provides essential insight into the physics underlying the interaction. A process which is providing access to the intricacies of the interaction is the generation of high order harmonics of the laser frequency. The phase-amplitude distribution of the emitted extreme-ultraviolet (EUV), carries the complete information about the harmonic generation process and vice-versa. Thus, the visualization of the EUV-spatial-amplitude-distribution, as it results from interfering electron wave-packet contributions, is of crucial importance. Restrictions to this accomplishment are due to the spatially integrating measurement approaches applied so far, that average out the phase effects in the generation process. In this work, we demonstrate a method which overcomes this obstacle. An EUV-spatial-amplitude-distribution-image is induced from the imprint on the measured spatial distribution of ions, produced through EUV-photon ionization of atoms. Interference extremes in the image carry phase information about the interfering electron wave-packets. The present approach provides detailed insight on the strong-field laser-atom interaction mechanism, while establishing the era of phase selective interaction studies. Furthermore, it paves the way for substantial enhancement of the spectral and temporal precision of measurements by in-situ controlling the phase distribution of the emitted radiation and/or spatially selecting the EUV-radiation-atom interaction products., Comment: 13 pages main text with 4 figures, 7 pages supporting material with 3 figures

The mass spectra for both horizontal and vertical polarizations and the angular distributions of fragment ions arising from Coulomb explosion of tetrahedral methyl iodide (CH3I) ions, obtained at a laser intensity of 1016 W cm-2 are presented. All fragment ion distributions are peaked along the direction corresponding to collinearity of the laser electric field with the time-of-flight mass spectrometer axis. The In + ion (n≤7) angular distributions from the dissociation of the parent ions are all of similar widths, which would imply a geometric, as opposed to dynamic, alignment. Additionally, the lower-charged I ions have an isotropic component that decreases as the charge state increases. Measurements of the CHm+ (m≤3), Cp + (p≤4) and H+ ion distributions show that these are also maximal along the polarization direction. Furthermore, there is also a CH22+ ion peak present in the CHm group, which has a distribution similar to those measured for the other ions. This mass peak is the prominent multi-charged ion in this group. As the CH3I molecule is initially tetrahedral, these results suggest that the molecular structure undergoes a change such that the H-C and C-I bonds tend to lie along the field. Several authors have described work which first aligned CH3I molecules with a nanosecond laser and then photodissociated with a femtosecond laser, to produce fragment ion distributions. This is the first time that the angular distributions from a tetrahedral molecule have been presented using femtosecond laser pulses only and in the case of CH3I, for fragments other than CH3+ and I+. The fragment energetics from the single CH3I molecule have been compared with those from recent work dealing with the Coulomb explosion of CH3I clusters.