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The generation of terawatt (TW) near-single-cycle laser pulses is of high interest for applications including attosecond science. Here we demonstrate a three-stage post-compression scheme in a non-guided geometry using He as the nonlinear medium, resulting in the generation of multi-mJ pulses with a duration of 3.7 fs. Key features of this approach are its simplicity, robustness and high stability, making it ideally suited for highly demanding applications such as attosecond-pump attosecond-probe spectroscopy (APAPS). This is demonstrated by performing two-color APAPS in Ar and Ne, where both simultaneous and sequential two-photon absorption are observed. Our approach is scalable to multi-TW powers., Comment: 9 pages, 4 figures

Extreme-ultraviolet (XUV) sources including high-harmonic generation, free-electron lasers, soft x-ray lasers and laser-driven plasmas are widely used for applications ranging from femtochemistry and attosecond science to coherent diffractive imaging and EUV lithography. The bandwidth of the XUV light emitted by these sources reflects the XUV generation process used. While light from soft-x-ray lasers and XUV FELs typically has a relatively narrow bandwidth, plasma sources and HHG sources driven by few-cycle laser pulses emit broadband XUV pulses. Since these characteristic properties of a given XUV source impose limitations to applications, techniques enabling modification of the XUV bandwidth are highly desirable. Here we demonstrate a concept for efficient spectral compression of a broadband XUV pulse via four-wave mixing (FWM) in the presence of a broadband near-infrared (NIR) pulse in a krypton gas jet, exploiting a phase-matching scheme based on closely-spaced resonances. Our concept provides new possibilities for tailoring the spectral bandwidth of XUV beams., Comment: 5 pages, 4 figures

Kerr-type nonlinearities form the basis for our physical understanding of nonlinear optical phenomena in condensed matter, such as self-focusing, solitary waves, and wave mixing. In strong fields, they are complemented by higher-order nonlinearities that enable high harmonic generation, which is currently understood as the interplay of light-driven intraband charge dynamics and interband recombination. Remarkably, the nonlinear response emerging from the associated sub-cycle injection dynamics of electrons into the conduction band has been almost completely overlooked in solids and only partially considered in the gas phase. Here we reveal this strong-field-induced nonlinearity in amorphous wide-bandgap dielectrics by means of time-resolved, low-order wave mixing experiments and show that close to the material damage threshold the so far unexplored injection current provides the leading contribution. The sensitivity of the harmonic emission to the sub-cycle ionization dynamics offers an original approach to characterize the evolution of laser-induced plasma formation in optical microprocessing., Comment: 14 pages, 4 figures

Recently two emerging areas of research, attosecond and nanoscale physics, have started to come together. Attosecond physics deals with phenomena occurring when ultrashort laser pulses, with duration on the femto- and sub-femtosecond time scales, interact with atoms, molecules or solids. The laser-induced electron dynamics occurs natively on a timescale down to a few hundred or even tens of attoseconds, which is comparable with the optical field. On the other hand, the second branch involves the manipulation and engineering of mesoscopic systems, such as solids, metals and dielectrics, with nanometric precision. Although nano-engineering is a vast and well-established research field on its own, the merger with intense laser physics is relatively recent. In this article we present a comprehensive experimental and theoretical overview of physics that takes place when short and intense laser pulses interact with nanosystems, such as metallic and dielectric nanostructures. In particular we elucidate how the spatially inhomogeneous laser induced fields at a nanometer scale modify the laser-driven electron dynamics. Consequently, this has important impact on pivotal processes such as ATI and HHG. The deep understanding of the coupled dynamics between these spatially inhomogeneous fields and matter configures a promising way to new avenues of research and applications. Thanks to the maturity that attosecond physics has reached, together with the tremendous advance in material engineering and manipulation techniques, the age of atto-nano physics has begun, but it is in the initial stage. We present thus some of the open questions, challenges and prospects for experimental confirmation of theoretical predictions, as well as experiments aimed at characterizing the induced fields and the unique electron dynamics initiated by them with high temporal and spatial resolution., Comment: Invited Review ROPP, 50 pages, 38 figures

We report on the characterization of space-time couplings in high energy sub-2-cycle 770nm laser pulses using a self-referencing single-shot method. Using spatially-encoded arrangement filter-based spectral phase interferometry for direct electric field reconstruction (SEA-F-SPIDER) we characterize few-cycle pulses with a wave-front rotation of 2.8x?10^11 rev/sec (1.38 mrad per half-cycle) and pulses with pulse front tilts ranging from to -0.33 fs/um to -3.03 fs/um., Comment: 6 pages, 6 figures

Attosecond streaking of photoelectrons emitted by extreme ultraviolet light has begun to reveal how electrons behave during their transport within simple crystalline solids. Many sample types within nanoplasmonics, thin-film physics, and semiconductor physics, however, do not have a simple single crystal structure. The electron dynamics which underpin the optical response of plasmonic nanostructures and wide-bandgap semiconductors happen on an attosecond timescale. Measuring these dynamics using attosecond streaking will enable such systems to be specially tailored for applications in areas such as ultrafast opto-electronics. We show that streaking can be extended to this very general type of sample by presenting streaking measurements on an amorphous film of the wide-bandgap semiconductor tungsten trioxide, and on polycrystalline gold, a material that forms the basis of many nanoplasmonic devices. Our measurements reveal the near-field temporal structure at the sample surface, and photoelectron wavepacket temporal broadening consistent with a spread of electron transport times to the surface.

We report the generation and characterization of isolated attosecond XUV and VUV pulses generated simultaneously via HHG driven by few-cycle pulses using an in-line dual gas target system. One gas jet target was operated with Kr gas that optimized HHG in the 15-25 eV photon energy range (VUV), whilst the second gas jet target was operated in Ne gas to optimize the high harmonic generation around 90 eV (XUV). Appropriate filters were used to isolate the required spectral components to synthesize isolated pulses. Sn and In filters were used for the VUV region while a Zr filter was used for the XUV. We characterized both the XUV and VUV pulses independently using the attosecond streaking technique and the LSGPA retrieval algorithm obtaining a 1.7$\pm$0.2 fs pulse using the In filter and a 616$\pm$50 as pulse using Sn, while preserving a 266$\pm$10 as isolated XUV pulse.

Quasi-free field-driven electron trajectories are a key element of strong-field dynamics. Upon recollision with the parent ion, the energy transferred from the field to the electron may be released as attosecond duration XUV emission in the process of high harmonic generation (HHG). The conventional sinusoidal driver fields set limitations on the maximum value of this energy transfer, and it has been predicted that this limit can be significantly exceeded by an appropriately ramped-up cycleshape. Here, we present an experimental realization of such cycle-shaped waveforms and demonstrate control of the HHG process on the single-atom quantum level via attosecond steering of the electron trajectories. With our optimized optical cycles, we boost the field-ionization launching the electron trajectories, increase the subsequent field-to-electron energy transfer, and reduce the trajectory duration. We demonstrate, in realistic experimental conditions, two orders of magnitude enhancement of the generated XUV flux together with an increased spectral cutoff. This application, which is only one example of what can be achieved with cycle-shaped high-field light-waves, has farreaching implications for attosecond spectroscopy and molecular self-probing.