Thin-disk laser-pumped OPCPA system delivering 4.4 TW few-cycle pulses.

We present an optical parametric chirped pulse amplification (OPCPA) system delivering 4.4 TW pulses centered at 810 nm with a sub-9 fs duration and a carrier-envelope phase stability of 350 mrad. The OPCPA setup pumped by sub-10 ps pulses from two Yb:YAG thin-disk lasers at 100 Hz repetition rate is optimized for a high conversion-efficiency. The terawatt pulses of the OPCPA are utilized for generating intense extreme ultraviolet (XUV) pulses by high-order harmonic generation, achieving XUV pulse energies approaching the microjoule level.

THz streak camera performance for single-shot characterization of XUV pulses with complex temporal structures.

The THz-field-driven streak camera has proven to be a powerful diagnostic-technique that enables the shot-to-shot characterization of the duration and the arrival time jitter of free electron laser (FEL) pulses. Here we investigate the performance of three computational approaches capable to determine the duration of FEL pulses with complex temporal structures from single-shot measurements of up to three simultaneously recorded spectra. We use numerically simulated FEL pulses in order to validate the accuracy of the pulse length retrieval in average as well as in a single-shot mode. We discuss requirements for the THz field strength in order to achieve reliable results and compare our numerical study with the analysis of experimental data that were obtained at the FEL in Hamburg - FLASH.

Low-Energy Electron Emission in the Strong-Field Ionization of Rare Gas Clusters.

Clusters and nanoparticles have been widely investigated to determine how plasmonic near fields influence the strong-field induced energetic electron emission from finite systems. We focus on the contrary, i.e., the slow electrons, and discuss a hitherto unidentified low-energy structure (LES) in the photoemission spectra of rare gas clusters in intense near-infrared laser pulses. For Ar and Kr clusters we find, besides field-driven fast electrons, a robust and nearly isotropic emission of electrons with <4 eV kinetic energies that dominates the total yield. Molecular dynamics simulations reveal a correlated few-body decay process involving quasifree electrons and multiply excited ions in the nonequilibrium nanoplasma that results in a dominant LES feature. Our results indicate that the LES emission occurs after significant nanoplasma expansion, and that it is a generic phenomenon in intense laser nanoparticle interactions, which is likely to influence the formation of highly charged ions.

Ionization Avalanching in Clusters Ignited by Extreme-Ultraviolet Driven Seed Electrons.

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 is 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.

Bright attosecond soft X-ray pulse trains by transient phase-matching in two-color high-order harmonic generation.

We study two-color high-order harmonic generation in Neon with 790 nm and 1300 nm driving laser fields and observe an extreme-ultraviolet continuum that extends to photon energies of 160 eV. Using a 6-mm-long, high pressure gas cell, we optimize the HHG yield at high photon energies and investigate the effect of ionization and propagation under phase-matching conditions that allow us to control the temporal structure of the XUV emission. Numerical simulations that include the 3D propagation of the two-color laser pulse show that a bright isolated attosecond pulse with exceptionally high photon energies can be generated in our experimental conditions due to an efficient hybrid optical and phase-matching gating mechanism.

Compact realization of all-attosecond pump-probe spectroscopy.

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 to 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 in many laboratories and permits investigations of fundamental processes that are not accessible by other pump-probe techniques.

Electron wave packet sampling with laser-generated extreme ultraviolet and terahertz fields.

We report on transferring the concept of light-field streaking with intense terahertz fields from free-electron lasers to the laboratory scale. Utilizing a commercial laser system, synchronized 300 µm terahertz and 13 nm extreme ultraviolet pulses are generated by optical rectification and high harmonic generation, respectively. The terahertz fields are sufficiently strong to support electron wave packet sampling with a few fs resolution. The capability of this approach is demonstrated by measuring the duration of electron pulses formed by direct photoemission from a neon gas target.

Field-Induced Tunneling Ionization and Terahertz-Driven Electron Dynamics in Liquid Water.

Liquid water at ambient temperature displays ultrafast molecular motions and concomitant fluctuations of very strong electric fields originating from the dipolar H2O molecules. We show that such random intermolecular fields induce the tunnel ionization of water molecules, which becomes irreversible if an external terahertz (THz) pulse imposes an additional directed electric field on the liquid. Time-resolved nonlinear THz spectroscopy maps charge separation, transport, and localization of the released electrons on a few-picosecond time scale. The highly polarizable localized electrons modify the THz absorption spectrum and refractive index of water, a manifestation of a highly nonlinear response. Our results demonstrate how the interplay of local electric field fluctuations and external electric fields allows for steering charge dynamics and dielectric properties in aqueous systems.

Correlated electronic decay in expanding clusters triggered by intense XUV pulses from a Free-Electron-Laser.

Irradiation of nanoscale clusters and large molecules with intense laser pulses transforms them into highly-excited non- equilibrium states. The dynamics of intense laser-cluster interaction is encoded in electron kinetic energy spectra, which contain signatures of direct photoelectron emission as well as emission of thermalized nanoplasma electrons. In this work we report on a so far not observed spectrally narrow bound state signature in the electron kinetic energy spectra from mixed Xe core - Ar shell clusters ionized by intense extreme-ultraviolet (XUV) pulses from a free-electron-laser. This signature is attributed to the correlated electronic decay (CED) process, in which an excited atom relaxes and the excess energy is used to ionize the same or another excited atom or a nanoplasma electron. By applying the terahertz field streaking principle we demonstrate that CED-electrons are emitted at least a few picoseconds after the ionizing XUV pulse has ended. Following the recent finding of CED in clusters ionized by intense near-infrared laser pulses, our observation of CED in the XUV range suggests that this process is of general relevance for the relaxation dynamics in laser produced nanoplasmas.

Strong-field ionization of clusters using two-cycle pulses at 1.8 µm.

The interaction of intense laser pulses with nanoscale particles leads to the production of high-energy electrons, ions, neutral atoms, neutrons and photons. Up to now, investigations have focused on near-infrared to X-ray laser pulses consisting of many optical cycles. Here we study strong-field ionization of rare-gas clusters (103 to 105 atoms) using two-cycle 1.8 µm laser pulses to access a new interaction regime in the limit where the electron dynamics are dominated by the laser field and the cluster atoms do not have time to move significantly. The emission of fast electrons with kinetic energies exceeding 3 keV is observed using laser pulses with a wavelength of 1.8 µm and an intensity of 1 × 1015 W/cm2, whereas only electrons below 500 eV are observed at 800 nm using a similar intensity and pulse duration. Fast electrons are preferentially emitted along the laser polarization direction, showing that they are driven out from the cluster by the laser field. In addition to direct electron emission, an electron rescattering plateau is observed. Scaling to even longer wavelengths is expected to result in a highly directional current of energetic electrons on a few-femtosecond timescale.