Streaking Experiments Research Articles

High-harmonic generation from a flat liquid-sheet plasma mirror

High-harmonic radiation can be generated when an ultra-intense laser beam is reflected from an over-dense plasma, known as a plasma mirror. It is considered a promising technique for generating intense attosecond pulses in the extreme ultraviolet and X-ray wavelength ranges. However, a solid target used for the formation of the over-dense plasma is completely damaged by the interaction. Thus, it is challenging to use a solid target for applications such as time-resolved studies and attosecond streaking experiments that require a large amount of data. Here we demonstrate that high-harmonic radiation can be continuously generated from a liquid plasma mirror in both the coherent wake emission and relativistic oscillating mirror regimes. These results will pave the way for the development of bright, stable, and high-repetition-rate attosecond light sources, which can greatly benefit the study of ultrafast laser-matter interactions.

Retrieval of photoionization group delay in chirped-attosecond pulses photoelectron streaking experiments

Photoionization time delays have been investigated in many streaking experiments in which an extreme ultraviolet (XUV) attosecond pulse is used to ionize the target in the presence of a dressing infrared laser field. The discrepancies between the photoionization time delays thus experiment measured and those from many sophisticated theoretical simulations have generated a great deal of controversy in recent years. The difficulty of achieving an accuracy of the retrieved time delays comes from two facts: a so-called wavepacket approximation is introduced to construct the photoionization electron wavepacket, this approximation is invalid if atto-chirp of XUV is non-zero; the other one is that the lower sensitivity of the streaking spectra to the phase of the photoionization transition dipole. Here we present a time delay retrieval method born from our recently proposed ‘phase retrieval of broadband pulses auto correlation’ (PROBP-AC) technology to overcome above limitations. We carefully exam the validity of our method and make a few compare with some other common used retrieval codes, and the simulations demonstrate that more accurate results can be retrieved using PROBP AC. Based on the present method, the angular dependent photoionization time delays can also be retrieved. Our investigation casts doubts on the measured group time delays in previous streaking experiments. We also mention here that a single photoionization group time delay at the XUV peak energy is not enough to represent a complete photoemission process; instead, a fully characterization of the photoionization group time delay over the whole bandwidth of the wave packet is required.

Generation and characterization of isolated attosecond pulses at 100 kHz repetition rate

The generation of coherent light pulses in the extreme ultraviolet (XUV) spectral region with attosecond pulse durations constitutes the foundation of the field of attosecond science. Twenty years after the first demonstration of isolated attosecond pulses, they continue to be a unique tool enabling the observation and control of electron dynamics in atoms, molecules, and solids. It has long been identified that an increase in the repetition rate of attosecond light sources is necessary for many applications in atomic and molecular physics, surface science, and imaging. Although high harmonic generation (HHG) at repetition rates exceeding 100 kHz, showing a continuum in the cutoff region of the XUV spectrum, was already demonstrated in 2013, the number of photons per pulse was insufficient to perform pulse characterization via attosecond streaking, let alone to perform a pump-probe experiment. Here we report on the generation and full characterization of XUV attosecond pulses via HHG driven by near-single-cycle pulses at a repetition rate of 100 kHz. The high number of 10 6 XUV photons per pulse on target enables attosecond electron streaking experiments through which the XUV pulses are determined to consist of a dominant single attosecond pulse. These results open the door for attosecond pump-probe spectroscopy studies at a repetition rate 1 or 2 orders of magnitude above current implementations.

Retrieval of attosecond pulse ensembles from streaking experiments using mixed state time-domain ptychography

The electric field of attosecond laser pulses can be retrieved from laser-dressed photoionisation measurements, where electron wavepackets that result from single-photon ionisation by the attosecond pulse in the presence of a dressing field are produced. In case of fluctuating dressing laser and/or attosecond pulses, e.g. due to pulse-to-pulse fluctuations of the carrier envelope phase of the infrared laser pulse, commonly applied retrieval algorithms result in the erroneous extraction of the pulse fields. We present a mixed state time-domain ptychography algorithm for the retrieval of pulse ensembles from attosecond streaking experiments.

Attosecond pulse retrieval from noisy streaking traces with conditional variational generative network

Accurate characterization of an attosecond pulse from streaking trace is an indispensable step in studying the ultrafast electron dynamics on the attosecond scale. Conventional attosecond pulse retrieval methods face two major challenges: the ability to incorporate a complete physics model of the streaking process, and the ability to model the uncertainty of pulse reconstruction in the presence of noise. Here we propose a pulse retrieval method based on conditional variational generative network (CVGN) that can address both demands. Instead of learning the inverse mapping from a streaking trace to a pulse profile, the CVGN models the distribution of the pulse profile conditioned on a given streaking trace measurement, and is thus capable of assessing the uncertainty of the retrieved pulses. This capability is highly desirable for low-photon level measurement, which is typical in attosecond streaking experiments in the water window X-ray range. In addition, the proposed scheme incorporates a refined physics model that considers the Coulomb-laser coupling and photoelectron angular distribution in streaking trace generation. CVGN pulse retrievals under various simulated noise levels and experimental measurement have been demonstrated. The results showed high pulse reconstruction consistency for streaking traces when peak signal-to-noise ratio (SNR) exceeds 6, which could serve as a reference for future learning-based attosecond pulse retrieval.

Controlling backward-scattering photoelectron holography by attosecond streaking

We study the two-dimensional photoelectron momentum distribution in a synthesized field of an attosecond pulse and a weak infrared femtosecond pulse by solving the time-dependent Schr\odinger equation of He atoms. The photoelectron momentum spectra reveal fruitful interference structures. With a semiclassical model, we show that some of the photoelectron interference structures come from the interference between the direct and backward-scattering electron trajectories. Those backward-scattering electrons are freed by the attosecond pulse and then are hard rescattered with parent ions by the streaking infrared field. By changing the phase delay between the attosecond pulse and the infrared laser field, we find that two kinds of backward-scattering electron trajectories will contribute to the holographic pattern. We show that backward-scattering holography can be explored with attosecond streaking experiments.

Attosecond streaking metrology with isolated nanotargets

The development of attosecond metrology has enabled time-resolved studies on atoms, molecules, and (nanostructured) solids. Despite a wealth of theoretical work, attosecond experiments on isolated nanotargets, such as nanoparticles, clusters, and droplets have been lacking. Only recently, attosecond streaking metrology could be extended to isolated silica nanospheres, enabling real-time measurements of the inelastic scattering time in dielectric materials. Here, we revisit these experiments and describe the single-shot analysis of velocity-map images, which permits to evaluate the recorded number of electrons. Modeling of the recorded electron histograms allows deriving the irradiated nanoparticle statistics. Theoretically, we analyze the influence of the nanoparticle size on the field-induced delay, which is one of the terms contributing to the measured streaking delay. The obtained new insight into attosecond streaking experiments on nanoparticles is expected to guide wider implementation of the approach on other types of nanoparticles, clusters, and droplets.

A new method for accurate retrieval of atomic dipole phase or photoionization group delay in attosecond photoelectron streaking experiments

In recent years, attosecond streaking experiments have been used to extract the phase of photoionization dipole transition matrix element (or the photoionization group delay) in atoms, molecules and condensed materials. The most accurate retrieval method so far is based on the frequency-resolved optical gating for complete reconstruction of attosecond bursts (FROG-CRAB). However, the FROG-CRAB employs a number of approximations that would cause errors in the retrieved results. In this article, we applied our recently proposed attosecond pulse characterization method phase retrieval of broadband pulses (PROBP) to the retrieval of photoionization group delay difference between Ne() and Ne() ionization channels, and between Ar() and Ne() channels. Our simulations demonstrate that more accurate results can be retrieved using PROBP than using FROG-CRAB, and cast doubts on group delays reported in previous streaking measurements.

Angular anisotropy of time delay in XUV+IR photoionization ofH2+

We develop a novel technique for modeling of atomic and molecular ionization in superposition of XUV and IR fields with characteristics typical for attosecond streaking and RABBITT experiments. The method is based on solving the time-dependent Schr\"odinger equation in the coordinate frame expanding along with the photoelectron wave packet. The efficiency of the method is demonstrated by calculating angular anisotropy of photoemission time delay of the H$_2^+$ ion in a field configuration of recent RABBITT experiments.

Time delays in correlated photoemission processes

We theoretically study time-resolved two-photon double ionization (TPDI) of helium as probed by attosecond streaking. We review recent advances in the understanding of the photoelectric effect in the time domain and discuss the differences between one- and two-photon ionization, as well as one- and two-electron emission. We perform exact ab-initio simulations for attosecond streaking experiments in the sequential TPDI regime and compare the results to the two-electron Eisenbud-Wigner-Smith delay for the process. Our calculations directly show that the timing of the emission process sensitively depends on the energy sharing between the two outgoing electrons. In particular, we identify Fano-like interferences in the relative time delay of the two emitted electrons when the sequential ionization channel occurs via intermediate excited ionic (shake-up) states. Furthermore, we find that the photoemission time delays are only weakly dependent on the relative emission angle of the ejected electrons.

Attosecond photoscopy of plasmonic excitations.

We propose an experimental arrangement to image, with attosecond resolution, transient surface plasmonic excitations. The required modifications to state-of-the-art setups used for attosecond streaking experiments from solid surfaces only involve available technology. Buildup and lifetimes of surface plasmon polaritons can be extracted and local modulations of the exciting optical pulse can be diagnosed insitu.

Numerical Simulations of Attosecond Streaking Time Delays in Photoionization

We present results of numerical simulations and theoretical classical analysis of time delays with respect to the instant of ionization in a numerical streaking experiment. These results confirm our previous interpretation of the streaking time delay as a finite-range and field-weighted time delay. We show that in the streaking experiments the time delay strongly depends on the parameters of the streaking field. Consequently, the streaking time delay is accumulated over a finite range in space, which the emitted electron probes after its transition into the continuum until the streaking pulse ceases. Moreover, we confirm by results of our numerical simulations that the streaking time delay can be understood as a sum (or integral) over field-free time delays weighted by the relative instantaneous field strength during the propagation of the photoelectron.

Transferring the attoclock technique to velocity map imaging

Attosecond angular streaking measurements have revealed deep insights into the timing of tunnel ionization processes of atoms in intense laser fields. So far experiments of this type have been performed only with a cold-target recoil-ion momentum spectrometer (COLTRIMS). Here, we present a way to apply attosecond angular streaking experiments to a velocity map imaging spectrometer (VMIS) with few-cycle pulses at a repetition rate of 10 kHz and a high ionization yield per pulse. Three-dimensional photoelectron momentum distributions from strong-field ionization of helium with an elliptically polarized, sub-10-fs pulse were retrieved by tomographic reconstruction from the momentum space electron images and used for the analysis in the polarization plane.

Time delay in valence-shell photoionization of noble-gas atoms

We use the non-relativistic random phase approximation with exchange to perform calculations of valence shell photoionization of Ne, Ar, Kr and Xe from their respective thresholds to photon energy of 200 eV. The energy derivative of the complex phase of the photoionization matrix elements is converted to the photoelectron group delay that can be measured in attosecond streaking or two-photon transitions interference experiments. Comparison with reported time delay measurements in Ne and Ar at a few selected photon energies is made. Systematic mapping of time delay across a wide range of photon energies in several atomic targets allows to highlight important aspects of fundamental atomic physics that can be probed by attosecond time delay measurements.

Evidence for Chirped Auger-Electron Emission

Auger decay carries valuable information about the electronic structure and dynamics of atoms, molecules, and solids. Here we furnish evidence that under certain conditions Auger electrons are subject to an energetic chirp. The effect is disclosed in time-resolved streaking experiments on the Xe NOO and Kr MNN Auger decay using extreme-ultraviolet pulses from the free-electron laser in Hamburg as well as from a high-order harmonic laser source. The origin of this effect is found to be an exchange of energy between the Auger electron and an earlier emitted correlated photoelectron. The observed time-dependent spectral modulations are understood within an analytical model and confirmed by extensive computer simulations.

Versatile apparatus for attosecond metrology and spectroscopy

We present the AS-2 Attosecond Beamline at the Joint Laboratory for Attosecond Physics of the Max-Planck-Institut für Quantenoptik and Ludwig-Maximilians-Universität for time resolved pump/probe experiments with attosecond resolution. High harmonic generation and subsequent filtering of the generated extreme ultraviolet (XUV) continuum by means of metal filters and XUV multilayer mirrors serve for the generation of isolated attosecond laser pulses. After high harmonic generation, the remaining fundamental laser pulse is spatially separated from the attosecond XUV pulse, to what is to our knowledge for the first time, by means of a perforated mirror in a Mach-Zehnder interferometer. Active stabilization of this interferometer guarantees the necessary temporal resolution for tracking attosecond dynamics in real time. As a proof-of-principle, photoelectron streaking experiments are performed and experimental techniques for their realization are summarized. Finally we highlight the potential of the presented beamline system for future experiments in comparison with previously demonstrated attosecond beamlines.

Calculations of the double differential cross section for attosecond laser-assisted photoionization of atoms

The energy and angular distributions of photoelectrons (the double differential cross sections, DDCS) for attosecond-pulse induced photoemission from atoms in the presence of a strong laser field are theoretically considered. We suggest a comparatively simple computational method based on the strong field approximation for calculation of the DDCS of short pulse photoionization which explicitly includes competing processes of interference and dephasing of the electronic wave packets. The method can be useful for analysis of attosecond streaking experiments. It is tested by comparison with the exact quantum-mechanical computation based on a numerical solving of the time-dependent Schrödinger equation. An excellent agreement between the two computational methods is demonstrated in a wide range of the pulse durations.