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In the last few decades the development of ultrafast lasers has revolutionized our ability to gain insight into light-matter interactions. The appearance of few-cycle light sources available from the visible to the mid-infrared spectral range and the development of attosecond extreme ultraviolet and x-ray technologies provide for the first time the possibility to directly observe and control ultrafast electron dynamics in matter on their natural time scale. However, few-fs sources have hardly been available in the deep ultraviolet (DUV; 4-6 eV, 300-200 nm) and are unavailable in the vacuum ultraviolet (VUV; 6-12 eV, 200-100 nm) spectral range, corresponding to the photon energies required for valence excitation of atoms and molecules. Here, we generate VUV pulses with $\mu$J energy tunable between 160 and 190 nm via resonant dispersive wave emission during soliton self-compression in a capillary. We fully characterize the pulses in situ using frequency-resolved optical gating based on two-photon photoionization in noble gases. The measurements reveal that in most of the cases the pulses are shorter than 3 fs. These findings unlock the potential to investigate ultrafast electron dynamics with a time-resolution that has been hitherto inaccessible when using VUV pulses.

The ability to perform attosecond-pump attosecond-probe spectroscopy (APAPS) is a longstanding goal in ultrafast science. While first pioneering experiments demonstrated the feasibility of APAPS, the low repetition rates (10-120 Hz) and the large footprints of existing setups have so far hindered the widespread exploitation of APAPS. Here we demonstrate two-color APAPS using a commercial laser system at 1 kHz, straightforward post-compression in a hollow-core fiber and a compact high-harmonic generation (HHG) setup. The latter enables the generation of intense extreme-ultraviolet (XUV) pulses by using an out-of-focus HHG geometry and by exploiting a transient blueshift of the driving laser in the HHG medium. Near-isolated attosecond pulses are generated, as demonstrated by one-color and two-color XUV-pump XUV-probe experiments. Our concept allows selective pumping and probing on extremely short timescales and permits investigations of fundamental processes that are not accessible by other pump-probe techniques., Comment: 8 pages, 5 figures

The generation of high-order harmonics in bulk solids subjected to intense ultrashort laser pulses has opened up new avenues for research in extreme nonlinear optics and light-matter interaction on sub-cycle timescales. Despite significant advancement over the past decade, a complete understanding of the involved phenomena is still lacking. High-harmonic generation in solids is currently understood as arising from nonlinear intraband currents, interband recollision and ionization-related phenomena. As all of these mechanisms involve or rely upon laser-driven excitation we combine measurements of the angular dependence of nonlinear absorption and high-order harmonic generation in bulk crystals to demonstrate the relation between high-harmonic emission and nonlinear, laser-induced ionization in solids. An unambiguous correlation between the emission of harmonics and laser-induced ionization is found experimentally, that is supported by numerical solutions of the semiconductor Bloch equations and calculations of orientation-dependent ionization rates using maximally localized Wannier-functions.

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 cut-off region of the XUV spectrum was already demonstrated in 2013, the number of photons per pulse was insufficient to perform pulse characterisation via attosecond streaking, let alone to perform a pump-probe experiment. Here we report on the generation and full characterisation 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 one or two orders of magnitude above current implementations., Comment: 27 Pages, 4 figures, supplementary information

The formation of an electron-hole plasma during the interaction of intense femtosecond laser pulses with transparent solids lies at the heart of femtosecond laser processing. Advanced micro- and nanomachining applications require improved control over the excitation characteristics. Here, we relate the emission of low-order harmonics to the strong laser-field-induced plasma formation. Together with a measurement of the total plasma density we identify the contribution of two competing ionization mechanisms - strong-field and electron-impact ionization.

High-intensity laser pulses covering the ultraviolet to terahertz spectral regions are nowadays routinely generated in a large number of laboratories. In contrast, intense extreme-ultraviolet (XUV) pulses have only been demonstrated using a small number of sources including free-electron laser facilities [1-3] and long high-harmonic generation (HHG) beamlines [4-9]. Here we demonstrate a concept for a compact intense XUV source based on HHG that is focused to an intensity of $2 \times 10^{14}$ W/cm$^2$, with a potential increase up to $10^{17}$ W/cm$^2$ in the future. Our approach uses tight focusing of the near-infrared (NIR) driving laser and minimizes the XUV virtual source size by generating harmonics several Rayleigh lengths away from the NIR focus. Accordingly, the XUV pulses can be refocused to a small beam waist radius of 600 nm, enabling the absorption of up to four XUV photons by a single Ar atom in a setup that fits on a modest (2 m) laser table. Our concept represents a straightforward approach for the generation of intense XUV pulses in many laboratories, providing novel opportunities for XUV strong-field and nonlinear optics experiments, for XUV-pump XUV-probe spectroscopy and for the coherent diffractive imaging of nanoscale structures., Comment: 6 pages, 4 figures

The development of schemes for coherent nonlinear time-domain spectroscopy in the extreme-ultraviolet regime (XUV) has so far been impeded by experimental difficulties that arise at these short wavelengths. In this work we present a novel experimental approach, which facilitates the timing control and phase cycling of XUV pulse sequences produced by harmonic generation in rare gases. The method is demonstrated for the generation and high spectral resolution characterization of narrow-bandwidth harmonics ($\approx14\,$eV) in argon and krypton. Our technique simultaneously provides high phase stability and a pathway-selective detection scheme for nonlinear signals - both necessary prerequisites for all types of coherent nonlinear spectroscopy., Comment: This is the accepted version of the article. The Version of Record is available online at 10.1088/1367-2630/abb43a

We report on the generation of 6.1 mJ, 3.8 fs pulses by the compression of a kHz Ti:sapphire laser in a large-aperture long hollow fiber. In order to find optimal conditions for spectral broadening at high pulse energies, we explore different parameter ranges where ionization or the Kerr effect dominates. After identifying the optimum parameter settings, large spectral broadening at high waveguide transmission is obtained. The intense 1.5-cycle pulses are used for high-harmonic generation in argon and neon.

Intense extreme-ultraviolet (XUV) pulses enable the investigation of XUV-induced nonlinear processes and are a prerequisite for the development of attosecond pump - attosecond probe experiments. While highly nonlinear processes in the XUV range have been studied at free-electron lasers (FELs), high-harmonic generation (HHG) has allowed the investigation of low-order nonlinear processes. Here we suggest a concept to optimize the HHG intensity, which surprisingly requires a scaling of the experimental parameters that differs substantially from optimizing the HHG pulse energy. As a result, we are able to study highly nonlinear processes in the XUV range using a driving laser with a modest ($\approx 10$ mJ) pulse energy. We demonstrate our approach by ionizing Ar atoms up to Ar$^{5+}$, requiring the absorption of at least 10 XUV photons., Comment: 11 pages, 4 figures

Many experiments in attosecond science will benefit from attosecond pulses at high repetition rates with sufficient photon flux for pump-probe experiments. We use 7fs, 800nm pulses from a non-collinear optical parametric chirped pulse amplification (NOPCPA) laser system to generate few-pulse attosecond pulse trains (APTs) in the extreme ultraviolet (XUV) at a repetition rate of 100kHz. The pulse trains have been fully characterized by recording FROG-CRAB (Frequency-Resolved Optical Gating for Complete Reconstruction of Attosecond Bursts) traces with a velocity map imaging spectrometer., Comment: 7 pages, 4 figures, submitted version

The strong coupling between intense laser fields and valence electrons in molecules causes a distortion of the potential energy hypersurfaces which determine the motion of nuclei in a molecule and influences possible reaction pathways. The coupling strength varies with the angle between the light electric field and valence orbital, and thereby adds another dimension to the effective molecular potential energy surface, allowing for the emergence of light-induced conical intersections. Here, we demonstrate in theory and experiment that the full complexity of such light-induced potential energy surfaces can be uncovered. In H$_2^+$, the simplest of molecules, we observe a strongly modulated angular distribution of protons which has escaped prior observation. These modulations directly result from ultrafast dynamics on the light-induced molecular potentials and can be modified by varying the amplitude, duration and phase of the mid-infrared dressing field. This opens new opportunities for manipulating the dissociation of small molecules using strong laser fields.

Direct laser writing of surface waveguides with ultrashort pulses is a crucial achievement towards all-laser manufacturing of photonic integrated circuits sensitive to their environment. In this Letter, few-cycle laser pulses (with a sub-10 fs duration) are used to produce subsurface waveguides in a non-doped, non-coated fused silica substrate. The fabrication technique relies on laser-induced microdensification below the threshold for nanopore formation. The optical losses of the fabricated waveguides are governed by the optical properties of the superstrate. We have measured losses ranging from less than 0.1~dB/mm (air superstrate) up to 2.8~dB/mm when immersion oil is applied on top of the waveguide.

We present a 100 kHz optical parametric chirped pulse amplifier (OPCPA) developed for strong-field attosecond physics and soft-X-ray transient absorption experiments. The system relies on noncollinear potassium titanyl arsenate (KTA) booster OPCPAs and is pumped by a 240 W, 1.1 ps Yb:YAG Innoslab chirped pulse laser amplifier. Two optically synchronized infrared output beams are simultaneously available: a 430 {\mu}J, 51 fs, carrier-envelope phase (CEP) stable beam at 1.55 {\mu}m and an angular-dispersion-compensated, 125 {\mu}J, 73 fs beam at 3.1 {\mu}m.

Refraction is a well-known optical phenomenon that alters the direction of light waves propagating through matter. Microscopes, lenses and prisms based on refraction are indispensable tools for controlling the properties of light beams at visible, infrared, ultraviolet and X-ray wavelengths. The large absorption of extreme-ultraviolet (XUV) radiation in matter, however, hinders the development of refractive lenses and prisms in this spectral region. Here, we demonstrate control over the refraction of XUV radiation by using a gas jet with a density gradient across the XUV beam profile. A gas phase prism is demonstrated that leads to a frequency-dependent deflection of the XUV beam. The strong deflection in the vicinity of atomic resonances is further used to develop a deformable XUV refractive lens, with low absorption and a focal length that can be tuned by varying the gas pressure. Our results provide novel opportunities in XUV science and open a route towards the transfer of refraction-based techniques including microscopy and nanofocusing, which are well established in other spectral regions, to the XUV domain., Comment: 8 pages, 4 figures

Coherent diffractive imaging of individual free nanoparticles has opened novel routes for the in-situ analysis of their transient structural, optical, and electronic properties. So far, single-shot single-particle diffraction was assumed to be feasible only at extreme ultraviolet (XUV) and X-ray free-electron lasers, restricting this research field to large-scale facilities. Here we demonstrate single-shot imaging of isolated helium nanodroplets using XUV pulses from a femtosecond-laser driven high harmonic source. We obtain bright wide-angle scattering patterns, that allow us to uniquely identify hitherto unresolved prolate shapes of superfluid helium droplets. Our results mark the advent of single-shot gas-phase nanoscopy with lab-based short-wavelength pulses and pave the way to ultrafast coherent diffractive imaging with phase-controlled multicolor fields and attosecond pulses.

An autoionizing resonance in molecular N$_2$ is excited by an ultrashort XUV pulse and probed by a subsequent weak IR pulse, which ionizes the contributing Rydberg states. Time- and angular-resolved photoelectron spectra recorded with a velocity map imaging spectrometer reveal two electronic contributions with different angular distributions. One of them has an exponential decay rate of $20\pm5$ fs, while the other one is shorter than 10 fs. This observation is interpreted as a manifestation of interference stabilization involving the two overlapping discrete Rydberg states. A formalism of interference stabilization for molecular ionization is developed and applied to describe the autoionizing resonance. The results of calculations reveal, that the effect of the interference stabilization is facilitated by rotationally-induced couplings of electronic states with different symmetry., Comment: 8 pages, 6 figures

We present the design, implementation and alignment procedure for a two-stage time delay compensating monochromator. The setup spectrally filters the radiation of a high-order harmonic generation source providing wavelength-selected XUV pulses with a bandwidth of 300 to 600~meV in the photon energy range of 3 to 50~eV. XUV pulses as short as $12\pm3$~fs are demonstrated. Transmission of the 400~nm (3.1~eV) light facilitates precise alignment of the monochromator. This alignment strategy together with the stable mechanical design of the motorized beamline components enables us to automatically scan the XUV photon energ in pump-probe experiments that require XUV beam pointing stability. The performance of the beamline is demonstrated by the generation of IR-assisted sidebands in XUV photoionization of argon atoms.

We study the ionization dynamics of Ar clusters exposed to ultrashort near-infrared (NIR) laser pulses for intensities well below the threshold at which tunnel ionization ignites nanoplasma formation. We find that the emission of highly charged ions up to Ar$^{8+}$ can be switched on with unit contrast by generating only a few seed electrons with an ultrashort extreme ultraviolet (XUV) pulse prior to the NIR field. Molecular dynamics simulations can explain the experimental observations and predict a generic scenario where efficient heating via inverse bremsstrahlung and NIR avalanching are followed by resonant collective nanoplasma heating. The temporally and spatially well-controlled injection of the XUV seed electrons opens new routes for controlling avalanching and heating phenomena in nanostructures and solids, with implications for both fundamental and applied laser-matter science., Comment: 5 pages, 4 figures