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Electrons photoemitted by extreme ultraviolet attosecond pulses derive spatially from the first few atomic surface layers and energetically from the valence band and highest atomic orbitals. As a result, it is possible to probe the emission dynamics from a narrow two-dimensional region in the presence of optical fields as well as obtain elemental specific information. However, combining this with spatially-resolved imaging is a long-standing challenge because of the large inherent spectral width of attosecond pulses as well as the difficulty of making them at high repetition rates. Here we demonstrate an attosecond interferometry experiment on a zinc oxide (ZnO) surface using spatially and energetically resolved photoelectrons. We combine photoemission electron microscopy with near-infrared pump - extreme ultraviolet probe laser spectroscopy and resolve the instantaneous phase of an infrared field with high spatial resolution. Our results show how the core level states with low binding energy of ZnO are well suited to perform spatially resolved attosecond interferometry experiments. We observe a distinct phase shift of the attosecond beat signal across the laser focus which we attribute to wavefront differences between the pump and the probe fields at the surface. Our work demonstrates a clear pathway for attosecond interferometry with high spatial resolution at atomic scale surface regions opening up for a detailed understanding of nanometric light-matter interaction.

The dispersion scan (d-scan) technique has emerged as a simple-to-implement characterization method for ultrashort laser pulses. D-scan traces are intuitive to interpret and retrieval algorithms that are both fast and robust have been developed to obtain the spectral phase and the temporal pulse profile. Here, we give a review of the d-scan technique based on second harmonic generation. We describe and compare recent implementations for the characterization of few- and multi-cycle pulses as well as two different approaches for recording d-scan traces in single-shot, thus showing the versatility of the technique., Comment: 16 pages, 7 figures

Attosecond pulses, produced through high-order harmonic generation in gases, have been successfully used for observing ultrafast, sub-femtosecond electron dynamics in atoms, molecules and solid state systems. Today's typical attosecond sources, however, are often impaired by their low repetition rate and the resulting insufficient statistics, especially when the number of detectable events per shot is limited. This is the case for experiments where several reaction products must be detected in coincidence, and for surface science applications where space-charge effects compromise spectral and spatial resolution. In this work, we present an attosecond light source operating at 200 kHz, which opens up the exploration of phenomena previously inaccessible to attosecond interferometric and spectroscopic techniques. Key to our approach is the combination of a high repetition rate, few-cycle laser source, a specially designed gas target for efficient high harmonic generation, a passively and actively stabilized pump-probe interferometer and an advanced 3D photoelectron/ion momentum detector. While most experiments in the field of attosecond science so far have been performed with either single attosecond pulses or long trains of pulses, we explore the hitherto mostly overlooked intermediate regime with short trains consisting of only a few attosecond pulses.e also present the first coincidence measurement of single-photon double ionization of helium with full angular resolution, using an attosecond source. This opens up for future studies of the dynamic evolution of strongly correlated electrons., Comment: 11 pages, 8 figures

When an intense, few-cycle light pulse impinges on a dielectric or semiconductor material, the electric field will interact nonlinearly with the solid, driving a coherent current. An asymmetry of the ultrashort, carrier-envelope-phase-stable waveform results in a net transfer of charge, which can be measured by macroscopic electric contact leads. This effect has been pioneered with extremely short, single-cycle laser pulses at low repetition rate, thus limiting the applicability of its potential for ultrafast electronics. We investigate lightwave-driven currents in gallium nitride using few-cycle laser pulses of nearly twice the duration and at a repetition rate two orders of magnitude higher than in previous work. We successfully simulate our experimental data with a theoretical model based on interfering multiphoton transitions, using the exact laser pulse shape retrieved from dispersion-scan measurements. Substantially increasing the repetition rate and relaxing the constraint on the pulse duration marks an important step forward towards applications of lightwave-driven electronics., Comment: 10 pages, 4 figures, 33 references, submitted to Optica

When an atom or molecule absorbs a high-energy photon, an electron is emitted with a well-defined energy and a highly-symmetric angular distribution, ruled by energy quantization and parity conservation. These rules seemingly break down when small quantum systems are exposed to short and intense light pulses, which raise the question of their universality for the simplest case of the photoelectric effect. Here we investigate the photoionization of helium by a sequence of attosecond pulses in the presence of a weak infrared dressing field. We continuously control the energy and introduce an asymmetry in the emission direction of the photoelectrons, thus contradicting well established quantum-mechanical predictions. This control is possible due to an extreme temporal confinement of the light-matter interaction. Our work extends time-domain coherent control schemes to one of the fastest processes in nature, the photoelectric effect., Comment: 18 pages, 4 figures

Ultrafast processes in matter can be captured and even controlled by using sequences of few-cycle optical pulses, which need to be well characterized, both in amplitude and phase. The same degree of control has not yet been achieved for few-cycle extreme ultraviolet pulses generated by high-order harmonic generation in gases, with duration in the attosecond range. Here, we show that by varying the spectral phase and carrier-envelope phase (CEP) of a high-repetition rate laser, using dispersion in glass, we achieve a high degree of control of the relative phase and CEP between consecutive attosecond pulses. The experimental results are supported by a detailed theoretical analysis based upon the semiclassical three-step model for high-order harmonic generation., Comment: 17 pages, 8 figures, published on 16 January 2018

We present efficient high-order harmonic generation (HHG) based on a high-repetition rate, few-cycle, near infrared (NIR), carrier-envelope phase stable, optical parametric chirped pulse amplifier (OPCPA), emitting 6fs pulses with 9{\mu}J pulse energy at 200kHz repetition rate. In krypton, we reach conversion efficiencies from the NIR to the extreme ultraviolet (XUV) radiation pulse energy on the order of ~10^{-6} with less than 3{\mu}J driving pulse energy. This is achieved by optimizing the OPCPA for a spatially and temporally clean pulse and by a specially designed high-pressure gas target. In the future, the high efficiency of the HHG source will be beneficial for high-repetition rate two-colour (NIR-XUV) pumpprobe experiments, where the available pulse energy from the laser has to be distributed economically between pump and probe pulses., Comment: 25 pages, 11 figures