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Within the last two decades attosecond science has been established as a novel research field providing insights into the ultrafast electron dynamics that follows a photoexcitation or photoionization process. Enabled by technological advances in ultrafast laser amplifiers, attosecond science has been in turn, a powerful engine driving the development of novel sources of intense ultrafast laser pulses. This article focuses on the development of high repetition rate laser-based sources delivering high energy pulses with a duration of only a few optical cycles, for applications in attosecond science. In particular, a high power, high repetition rate optical parametric chirped pulse amplification system is described, which was developed to drive an attosecond pump-probe beamline targeting photoionization experiments with electron-ion coincidence detection at high acquisition rates.

We present a new methodology for measuring few-femtosecond electronic and nuclear dynamics in both atoms and polyatomic molecules using multidimensional high harmonic generation (HHG) spectroscopy measurements, in which the spectra are recorded as a function of the laser intensity to form a two-dimensional data set. The method is applied to xenon atoms and to benzene molecules, the latter exhibiting significant fast nuclear dynamics following ionization. We uncover the signature of the sub-cycle evolution of the returning electron flux in strong-field ionized xenon atoms, implicit in the strong field approximation but not previously observed directly. We furthermore extract the nuclear autocorrelation function in strong field ionized benzene cations, which is determined to have a decay of $$\tau _0 = 4 \pm 1$$ τ 0 = 4 ± 1 fs, in good agreement with the $$ \tau _0 = 3.5$$ τ 0 = 3.5 fs obtained from direct dynamics variational multi-configuration Gaussian calculations. Our method requires minimal assumptions about the system, and is applicable even to un-aligned polyatomic molecules.

We study propagation effects due to the finite speed of light in ionization of extended molecular systems. We present a general quantitative theory of these effects and show under which conditions such effects should appear. The finite speed of light propagation effects are encoded in the non-dipole terms of the time-dependent Shrödinger equation and display themselves in the photoelectron momentum distribution projected on the molecular axis. Our numerical modeling for the $$\hbox {H}_{2}^{+}$$ H 2 + molecular ion and the $$\hbox {Ne}_2$$ Ne 2 dimer shows that the finite light propagation time from one atomic center to another can be accurately determined in a table top laser experiment which is much more readily accessible than the ground breaking synchrotron measurement by Grundmann et al. (Science 370:339, 2020).

Capturing electronic dynamics in real time has been the ultimate goal of attosecond science since its beginning. While for atomic targets the existing measurement techniques have been thoroughly validated, in molecules there are open questions due to the inevitable copresence of moving nuclei, which are not always mere spectators of the phototriggered electron dynamics. Previous work has shown that not only can nuclear motion affect the way electrons move in a molecule, but it can also lead to contradictory interpretations depending on the chosen experimental approach. In this Letter we investigate how nuclear motion affects and eventually distorts the electronic dynamics measured by using two of the most popular attosecond techniques, reconstruction of attosecond beating by interference of two-photon transitions and attosecond streaking. Both methods are employed, in combination with ab initio theoretical calculations, to retrieve photoionization delays in the dissociative ionization of H2, H2→H?, in the region of the Q1 series of autoionizing states, where nuclear motion plays a prominent role. We find that the experimental reconstruction of attosecond beating by interference of two-photon transitions results are very sensitive to bond softening around the Q1 threshold (27.8 eV), even at relatively low infrared (IR) intensity (I0∼1.4×1011 W/cm2), due to the long duration of the probe pulse that is inherent to this technique. Streaking, on the other hand, seems to be a better choice to isolate attosecond electron dynamics, since shorter pulses can be used, thus reducing the role of bond softening. This conclusion is supported by very good agreement between our streaking measurements and the results of accurate theoretical calculations. Additionally, the streaking technique offers the necessary energy resolution to accurately retrieve the fast-oscillating phase of the photoionization matrix elements, an essential requirement for extending this technique to even more complicated molecular targets., Physical Review Letters, 128 (6), ISSN:0031-9007, ISSN:1079-7114

Free-electron lasers (FELs) can produce radiation in the short wavelength range extending from the extreme ultraviolet (XUV) to the X-rays with a few to a few tens of femtoseconds pulse duration. These facilities have enabled significant breakthroughs in the field of atomic, molecular, and optical physics, implementing different schemes based on two-color photoionization mechanisms. In this article, we present the generation of attosecond pulse trains (APTs) at the seeded FEL FERMI using the beating of multiple phase-locked harmonics. We demonstrate the complex attosecond waveform shaping of the generated APTs, exploiting the ability to manipulate independently the amplitudes and the phases of the harmonics. The described generalized attosecond waveform synthesis technique with an arbitrary number of phase-locked harmonics will allow the generation of sub-100 as pulses with programmable electric fields.

Characterizing time delays in molecular photoionization as a function of the ejected electron emission direction relative to the orientation of the molecule and the light polarization axis provides unprecedented insights into the attosecond dynamics induced by extreme ultraviolet or X-ray one-photon absorption, including the role of electronic correlation and continuum resonant states. Here, we report completely resolved experimental and computational angular dependence of single-photon ionization delays in NO molecules across a shape resonance, relying on synchrotron radiation and time-independent ab initio calculations. The angle-dependent time delay variations of few hundreds of attoseconds, resulting from the interference of the resonant and non-resonant contributions to the dynamics of the ejected electron, are well described using a multichannel Fano model where the time delay of the resonant component is angle-independent. Comparing these results with the same resonance computed in e-NO+ scattering highlights the connection of photoionization delays with Wigner scattering time delays., It is an interesting topic to find the time it takes for an electron to escape an atom or a molecule after photoionization. Here the authors measure the angular dependence of photoionization time delay in the molecular frame and discuss the role of shape resonances.

Laser-assisted electron scattering (LAES), a light–matter interaction process that facilitates energy transfer between strong light fields and free electrons, has so far been observed only in gas phase. Here we report on the observation of LAES at condensed phase particle densities, for which we create nano-structured systems consisting of a single atom or molecule surrounded by a superfluid He shell of variable thickness (32–340 Å). We observe that free electrons, generated by femtosecond strong-field ionization of the core particle, can gain several tens of photon energies due to multiple LAES processes within the liquid He shell. Supported by Monte Carlo 3D LAES and elastic scattering simulations, these results provide the first insight into the interplay of LAES energy gain/loss and dissipative electron movement in a liquid. Condensed-phase LAES creates new possibilities for space-time studies of solids and for real-time tracing of free electrons in liquids., Laser-assisted electron scattering (LAES) is a commonly observed strong field process in gas phase systems. Here the authors use helium droplets with core atoms and molecules to observe increased electron energy due to multiple LAES events within the droplets.

Light beams with helical phase-fronts are known to carry orbital angular momentum (OAM) and provide an additional degree of freedom to beams of coherent light. While OAM beams can be readily derived from Gaussian laser beams with phase plates or gratings, this is far more challenging in the extreme ultra-violet (XUV), especially for the case of high XUV intensity. Here, we theoretically and numerically demonstrate that intense surface harmonics carrying OAM are naturally produced by the intrinsic dynamics of a relativistically intense circularly-polarized Gaussian beam (i.e. non-vortex) interacting with a target at normal incidence. Relativistic surface oscillations convert the laser pulses to intense XUV harmonic radiation via the well-known relativistic oscillating mirror mechanism. We show that the azimuthal and radial dependence of the harmonic generation process converts the spin angular momentum of the laser beam to orbital angular momentum resulting in an intense attosecond pulse (or pulse train) with OAM., Vortices in light fields are of growing importance in the XUV and X-ray ranges. Here the authors show by simulations that high harmonics and attosecond pulses, generated while irradiating a deformed thin foil with circularly-polarized Gaussian laser pulses, carry a well-defined orbital angular momentum.

The last decade has seen an intense renewed debate on tunnelling time, both from a theoretical and an experimental perspective. Here, we review recent developments and new insights in the field of strong-field tunnel ionization related to tunnelling time, and apply these findings to the interpretation of the attoclock experiment Landsman et al. [Optica 2014, 1, 343]. We conclude that models including finite tunnelling time are consistent with recent experimental measurements., Journal of Modern Optics, 66 (10), ISSN:0950-0340, ISSN:0030-3909, ISSN:1362-3044

Structured light, which exhibits nontrivial intensity, phase, and polarization patterns in space, has key applications ranging from imaging and 3D micromanipulation to classical and quantum communication. However, to date, its application to molecular chirality has been limited by the weakness of magnetic interactions. Here we structure light’s local handedness in space to introduce and realize an enantio-sensitive interferometer for efficient chiral recognition without magnetic interactions, which can be seen as an enantio-sensitive version of Young’s double slit experiment. Upon interaction with isotropic chiral media, such chirality-structured light effectively creates chiral emitters of opposite handedness, located at different positions in space. We show that if the distribution of light’s handedness breaks left-right symmetry, the interference of these chiral emitters leads to unidirectional bending of the emitted light, in opposite directions in media of opposite handedness, even if the number of the left-handed and right-handed emitters excited in the medium is exactly the same. Our work introduces the concepts of polarization of chirality and chirality-polarized light, exposes the immense potential of sculpting light’s local chirality, and offers novel opportunities for efficient chiral discrimination, enantio-sensitive optical molecular fingerprinting and imaging on ultrafast time scales., Developing new methods for structuring light’s chirality in space would be advantageous for various next-generation applications. Here, the authors report enantio-sensitive unidirectional light bending by interacting light with isotropic chiral media.

[EN] A controversy surrounding the “tunnelling time problem” stems from the seeming inability of quantum mechanics to provide, in the usual way, a definition of the duration a particle is supposed to spend in a given region of space. For this reason, the problem is often approached from an “operational” angle. Typically, one tries to mimic, in a quantum case, an experiment which yields the desired result for a classical particle. One such approach is based on the use of a Larmor clock. We show that the difficulty with applying a non-perturbing Larmor clock in order to “time” a classically forbidden transition arises from the quantum Uncertainty Principle. We also demonstrate that for this reason a Larmor time (in fact, any Larmor time) cannot be interpreted as a physical time interval. We provide a theoretical description of the quantities measured by the clock. Financial support of MCIU, through the grant PGC2018-101355-B-100(MCIU/AEI/FEDER,UE) (DS), and of the Basque Government through Grant No. IT986-16 (DS) is gratefully acknowledged. EA acknowledges the financial support of the Ministerio de Economía y Competitividad (MINECO) of the Spanish Government through BCAM Severo Ochoa accreditation SEV-2017-0718 and PID2019-104927GB-C22 grant. This work was also supported by the BERC 2018e2021 Program and ELKARTEK Programme (KK-2020/00049 and KK-2020/00008) funded by the Basque Government.

Attosecond science promises to reveal the most fundamental electronic dynamics occurring in matter and it can develop further by meeting two linked technological goals related to high-order harmonic sources: improved spectral tunability (allowing selectivity in addressing electronic transitions) and higher photon flux (permitting to measure low cross-section processes). New developments come through parametric waveform synthesis, which provides control over the shape of field transients, enabling the creation of highly-tunable isolated attosecond pulses via high-harmonic generation. Here we demonstrate that the first goal is fulfilled since central energy, spectral bandwidth/shape and temporal duration of isolated attosecond pulses can be controlled by shaping the laser waveform via two key parameters: the relative-phase between two halves of the multi-octave spanning spectrum, and the overall carrier-envelope phase. These results not only promise to expand the experimental possibilities in attosecond science, but also demonstrate coherent strong-field control of free-electron trajectories using tailored optical waveforms., Attosecond pulse generation needs improvements both in terms of tunability and photon flux for next level attosecond experiments. Here the authors show how to control the HHG emission and its spectral-temporal characteristics by driving the IAP generation with synthesized sub-cycle optical pulses.

More than 100 years after its discovery and its explanation in the energy domain, the duration of the photoelectric effect is still heavily studied. The emission time of a photoelectron can be quantified by the Wigner time delay. Experiments addressing this time delay for single-photon ionization became feasible during the last 10 years. A missing piece, which has not been studied, so far, is the Wigner time delay for strong-field ionization of molecules. Here we show experimental data on the Wigner time delay for tunnel ionization of $H_{2}$ molecules and demonstrate its dependence on the emission direction of the electron with respect to the molecular axis. We find, that the observed changes in the Wigner time delay can be quantitatively explained by elongated/shortened travel paths of the electrons that are due to spatial shifts of the electron's birth position after tunneling. This introduces an intuitive perspective towards the Wigner time delay in strong-field ionization., Comment: 17 pages, 6 figures

The Coulomb interaction between a photoelectron and its parent ion plays an important role in a large range of light-matter interactions. In this paper we obtain a direct insight into the Coulomb interaction and resolve, for the first time, the phase accumulated by the laser-driven electron as it interacts with the Coulomb potential. Applying extreme-ultraviolet interferometry enables us to resolve this phase with attosecond precision over a large energy range. Our findings identify a strong laser-Coulomb coupling, going beyond the standard recollision picture within the strong-field framework. Transformation of the results to the time domain reveals Coulomb-induced delays of the electrons along their trajectories, which vary by tens of attoseconds with the laser field intensity.

Time-resolved photoelectron spectroscopy with attosecond precision provides new insights into the photoelectric effect and gives information about the timing of photoemission from different electronic states within the electronic band structure of solids. Electron transport, scattering phenomena and electron-electron correlation effects can be observed on attosecond time scales by timing photoemission from valence band states against that from core states. However, accessing intraband effects was so far particularly challenging due to the simultaneous requirements on energy, momentum and time resolution. Here we report on an experiment utilizing intracavity generated attosecond pulse trains to meet these demands at high flux and high photon energies to measure intraband delays between sp- and d-band states in the valence band photoemission from tungsten and investigate final-state effects in resonant photoemission., Accessing intraband dynamics is challenging due to simultaneous requirements on energy, momentum and time resolution. Here, the authors measure intraband delays between sp- and d-band electronic states in the valence band photoemission from W(110) using intracavity generated attosecond pulse trains.

We present a compact experimental setup for performing attosecond-pump-infrared-probe experiments with long-time delay stability. The robustness of the setup is demonstrated over a two-day acquisition time in two-photon photoionization of argon in the photon-energy range 17−33 eV. The propagation of the input infrared pulse, as driving pulse for the high-order harmonic generation process and for the generation of the sidebands of the main photoelectron peaks, through the main optical components is simulated and discussed. Our setup allows us to perform attosecond experiments with an overall stability of ± 40 as.

New journal of physics 22(5), 053028 (1-9) (2020). doi:10.1088/1367-2630/ab83d7, Coherent, broadband pulses of extreme ultraviolet light provide a new and exciting tool for exploring attosecond electron dynamics. Using photoelectron streaking, interferometric spectrograms can be generated that contain a wealth of information about the phase properties of the photoionization process. If properly retrieved, this phase information reveals attosecond dynamics during photoelectron emission such as multielectron dynamics and resonance processes. However, until now, the full retrieval of the continuous electron wavepacket phase from isolated attosecond pulses has remained challenging. Here, after elucidating key approximations and limitations that hinder one from extracting the coherent electron wavepacket dynamics using available retrieval algorithms, we present a new method called absolute complex dipole transition matrix element reconstruction (ACDC). We apply the ACDC method to experimental spectrograms to resolve the phase and group delay difference between photoelectrons emitted from Ne and Ar. Our results reveal subtle dynamics in this group delay difference of photoelectrons emitted form Ar. These group delay dynamics were not resolvable with prior methods that were only able to extract phase information at discrete energy levels, emphasizing the importance of a complete and continuous phase retrieval technique such as ACDC. Here we also make this new ACDC retrieval algorithm available with appropriate citation in return., Published by IOP, [London]

Nature Communications 11(1), 3407 (2020). doi:10.1038/s41467-020-17250-0, Ultrafast, high-intensity light-matter interactions lead to optical-field-driven photocurrents with an attosecond-level temporal response. These photocurrents can be used to detect the carrier-envelope-phase (CEP) of short optical pulses, and enable optical-frequency, petahertz (PHz) electronics for high-speed information processing. Despite recent reports on optical-field-driven photocurrents in various nanoscale solid-state materials, little has been done in examining the large-scale electronic integration of these devices to improve their functionality and compactness. In this work, we demonstrate enhanced, on-chip CEP detection via optical-field-driven photocurrents in a monolithic array of electrically-connected plasmonic bow-tie nanoantennas that are contained within an area of hundreds of square microns. The technique is scalable and could potentially be used for shot-to-shot CEP tagging applications requiring orders-of-magnitude less pulse energy compared to alternative ionization-based techniques. Our results open avenues for compact time-domain, on-chip CEP detection, and inform the development of integrated circuits for PHz electronics as well as integrated platforms for attosecond and strong-field science., Published by Nature Publishing Group UK, [London]

This work presents a photodissociation study of the diamondoid adamantane using extreme ultraviolet femtosecond pulses. The fragmentation dynamics of the dication is unraveled by the use of advanced ion and electron spectroscopy giving access to the dissociation channels as well as their energetics. To get insight into the fragmentation dynamics, we use a theoretical approach combining potential energy surface determination, statistical fragmentation methods and molecular dynamics simulations. We demonstrate that the dissociation dynamics of adamantane dications takes place in a two-step process: barrierless cage opening followed by Coulomb repulsion-driven fragmentation, This research was supported by the Swedish Research Council, the Swedish Foundation for Strategic Research and the Crafoord Foundation. This project has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Grant Agreement No. 641789 MEDEA and under grant agreement no 654148 Laserlab-Europe. The research was conducted in the framework of the International Associated Laboratory (LIA) Fragmentation DYNAmics of complex MOlecular systems - DYNAMO, funded by the Centre National de la Recherche Scientifique (CNRS). The authors acknowledge the generous allocation of computer time at the Centro de Computación Científica at the Universidad Autónoma de Madrid (CCC-UAM). This work was partially supported by the project CTQ2016-76061-P of the Spanish Ministerio de Economía y Competitividad (MINECO). Financial support from the MINECO through the "María de Maeztu” Program for Units of Excellence in R&D (MDM-2014-0377) is also acknowledged

We report on the application of femtosecond laser micromachining to the fabrication of complex glass microdevices, for high-order harmonic generation in gas. The three-dimensional capabilities and extreme flexibility of femtosecond laser micromachining allow us to achieve accurate control of gas density inside the micrometer interaction channel. This device gives a considerable increase in harmonics&rsquo, generation efficiency if compared with traditional harmonic generation in gas jets. We propose different chip geometries that allow the control of the gas density and driving field intensity inside the interaction channel to achieve quasi phase-matching conditions in the harmonic generation process. We believe that these glass micro-devices will pave the way to future downscaling of high-order harmonic generation beamlines.

The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within an XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths., Light pulses with controllable parameters are desired for studying the fundamental properties of matter. Here the authors generate and use phase-manipulated and highly time-stable XUV pulse pairs to probe the coherent evolution and dephasing of XUV electronic coherences in helium and argon.

We study ultrafast ionization dynamics using orthogonally polarized two-color (OTC) laser pulses involving the resonant "first plus second" ($\omega+2\omega$) scheme. The scheme is illustrated by numerical simulations of the time-dependent Schr\"odinger equation and recording the photoelectron momentum distribution. On the basis of the simulations of this resonant ionization, we identify signatures of the dynamic Autler-Townes effect and dynamic interference, in which their characterization is not possible in spectral domain. Taking advantage of the OTC scheme we show that these dynamical effects, which occur at the same time scale, can be characterized in momentum space by controlling the spatial quantum interference. In particular, we show that with the use of this control scheme, one can tailor the properties of the control pulse to lead to enhancement of the ionization rate through the Autler-Townes effect without affecting the dynamic interference. This enhancement is shown to result from constructive interferences between partial photoelectron waves having opposite-parity, and found to manifest by symmetry-breaking of the momentum distribution. The scenario is investigated for a prototype of a hydrogen atom and is broadly applicable to other systems. Our findings may have applications for photoelectron interferometers to control the electron dynamics in time and space, and for accurate temporal characterization of attosecond pulses., Comment: 12 pages, 6 figures

An attosecond molecular interferometer is proposed by using a XUV–XUV pump-probe scheme. The interferograms resulting in the photoelectron distributions enable the full reconstruction of the molecular wave packet associated to excited states using a quantum state holographic approach that, to our knowledge, has only been proposed for simple atomic targets combining attosecond XUV pulses with IR light. In contrast with existing works, we investigate schemes where one- and two-photon absorption paths contribute to ionize the hydrogen molecule and show that it is possible to retrieve the excitation dynamics even when imprinted in a minority channel. Furthermore, we provide a systematic analysis of the time-frequency maps that reveal the distinct, but tightly coupled, motion of electrons and nuclei.

Transient absorption spectroscopy is utilized extensively for measurements of bound- and quasibound-state dynamics of atoms and molecules. The extension of this technique into the extreme ultraviolet (XUV) region with attosecond pulses has the potential to attain unprecedented time resolution. Here we apply this technique to aligned-in-space molecules. The XUV pulses are much shorter than the time during which the molecules remain aligned, typically \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$, Transient absorption spectroscopy is used to identify the structural characteristics of the atoms and molecules. Here the authors used extreme ultraviolet transient absorption spectroscopy to identify the Rydberg state symmetry of aligned molecules.