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 (1 attosecond=1 as=10 −18 s), which is comparable with the optical field. For comparison, the revolution of an electron on a 1s orbital of a hydrogen atom is ∼ 152 as. 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 report on progress 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 above-threshold ionization and high-order harmonic generation. 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.

The promise of ultrafast light-field-driven electronic nanocircuits has stimulated the development of the new research field of attosecond nanophysics. An essential prerequisite for advancing this new area is the ability to characterize optical near fields from light interaction with nanostructures, with sub-cycle resolution. Here we experimentally demonstrate attosecond near-field retrieval for a tapered gold nanowire. By comparison of the results to those obtained from noble gas experiments and trajectory simulations, the spectral response of the nanotaper near field arising from laser excitation can be extracted.

Laser-dressed photoelectron spectroscopy, employing extreme-ultraviolet attosecond pulses obtained by femtosecond-laser-driven high-order harmonic generation, grants access to atomic-scale electron dynamics. Limited by space charge effects determining the admissible number of photoelectrons ejected during each laser pulse, multidimensional (i.e. spatially or angle-resolved) attosecond photoelectron spectroscopy of solids and nanostructures requires high-photon-energy, broadband high harmonic sources operating at high repetition rates. Here, we present a high-conversion-efficiency, 18.4-MHz-repetition-rate cavity-enhanced high harmonic source emitting 5 × 105 photons per pulse in the 25-to-60-eV range, releasing 1 × 1010 photoelectrons per second from a 10-µm-diameter spot on tungsten, at space charge distortions of only a few tens of meV. Broadband, time-of-flight photoelectron detection with nearly 100% temporal duty cycle evidences a count rate improvement between two and three orders of magnitude over state-of-the-art attosecond photoelectron spectroscopy experiments under identical space charge conditions. The measurement time reduction and the photon energy scalability render this technology viable for next-generation, high-repetition-rate, multidimensional attosecond metrology.

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Ultrafast light-induced molecular reactions on aerosolized nanoparticles may elucidate early steps in the photoactivity of nanoparticles with potential impact in fields ranging from chemistry and medicine to climate science. In situ morphology discrimination for nanoparticle streams when measuring light-induced reaction yields is crucial, but lacking. Here, we experimentally demonstrate, using the reaction nanoscopy technique, that proton momenta from deprotonation reactions induced by intense femtosecond pulses exhibit clear, distinguishable signatures for single silica nanospheres and their clusters. Our findings are supported by classical trajectory Monte Carlo simulations. The results demonstrate an in situ single-shot discrimination method between reaction yields from photoinduced processes on single particles and their clusters. We find that the ionization of clusters dominates at sufficiently low intensities, providing an explanation to resolve previously observed discrepancies between experimental data and theoretical treatments, which considered only single nanoparticles.

Light-field driven electron localization in deuterium molecules in intense near single-cycle laser fields is studied as a function of the laser intensity. The emission of D + ions from the dissociative ionization of D 2 is interrogated with single-shot carrier-envelope phase (CEP)-tagged velocity map imaging. We explore the reaction for an intensity range of (1.0-2.8) × 10 14 W cm −2 , where laser-driven electron recollision leads to the population of excited states of D 2 +. Within this range we find the onset of dissociation from 3σ states of D 2+ by comparing the experimental data to quantum dynamical simulations including the first eight states of D 2 + . We find that dissociation from the 3σ states yields D + ions with kinetic energies above 8 eV. Electron localization in the dissociating molecule is identified through an asymmetry in the emission of D + ions with respect to the laser polarization axis. The observed CEP-dependent asymmetry indicates two mechanisms for the population of 3σ states: (1) excitation by electron recollision to the lower excited states, followed by laser-field excitation to the 3σ states, dominating at low intensities, and (2) direct excitation to the 3σ states by electron recollision, playing a role at higher intensities.

Isolated attosecond pulses (IAPs) produced through laser-driven high-harmonic generation (HHG) hold promise for unprecedented insight into physical, chemical, and biological processes via attosecond x-ray diffraction and spectroscopy with tabletop sources. Efficient scaling of HHG towards x-ray energies, however, has been hampered by ionization-induced plasma generation impeding the coherent buildup of high-harmonic radiation. Recently, it has been shown that these limitations can be overcome in the socalled "overdriven regime" where ionization loss and plasma dispersion strongly modify the driving laser pulse over small distances, albeit without demonstrating IAPs. Here, we report on experiments contrasting the generation of IAPs at 80 eV in argon with neon via attosecond streaking measurements. Comparing our experimental results to numerical simulations, we conclude that IAPs in argon are generated in the overdriven regime. We introduce a simple expression that fully describes the HHG dipole phase-mismatch contribution, specifically the effect of the blueshift of the driving laser. Furthermore, we present a method to numerically calculate the transient HHG phase mismatch, which allows us to demonstrate the accuracy of the introduced phase-mismatch expression. Finally, we perform simulations for different gases and wavelengths and show that including the full HHG dipole phase-mismatch contribution is important for understanding HHG with long-wavelength, few-cycle laser pulses in high-pressure gas targets, which are currently being employed for scaling isolated attosecond pulse generation beyond extreme ultraviolet (XUV) towards soft-x-ray photon energies.

Extreme nonlinear terahertz electro-optics in diamond for ultrafast pulse switching APL Photonics 2, 036106 (2017) Metal nanotip photoemitters have proven to be versatile in fundamental nanoplasmonics research and applications, including, e.g., the generation of ultrafast electron pulses, the adiabatic focusing of plasmons, and as light-triggered electron sources for microscopy. Here, we report the generation of high energy photoelectrons (up to 160 eV) in photoemission from single-crystalline nanowire tips in few-cycle, 750-nm laser fields at peak intensities of (2-7.3) × 10 12 W/cm 2 . Recording the carrier-envelope phase (CEP)-dependent photoemission from the nanowire tips allows us to identify rescattering contributions and also permits us to determine the high-energy cutoff of the electron spectra as a function of laser intensity. So far these types of experiments from metal nanotips have been limited to an emission regime with less than one electron per pulse. We detect up to 13 e/shot and given the limited detection efficiency, we expect up to a few ten times more electrons being emitted from the nanowire. Within the investigated intensity range, we find linear scaling of cutoff energies. The nonlinear scaling of electron count rates is consistent with tunneling photoemission occurring in the absence of significant charge interaction. The high electron energy gain is attributed to field-induced rescattering in the enhanced nanolocalized fields at the wires apex, where a strong CEP-modulation is indicative of the attosecond control of photoemission. © 2017 Author(s)