The local enhancement of few-cycle laser pulses by plasmonic nanostructures opens up for spatiotemporal control of optical interactions on a nanometer and few-femtosecond scale. However, spatially resolved characterization of few-cycle plasmon dynamics poses a major challenge due to the extreme length and time scales involved. In this Letter, we experimentally demonstrate local variations in the dynamics during the few strongest cycles of plasmon-enhanced fields within individual rice-shaped silver nanoparticles. This was done using 5.5 fs laser pulses in an interferometric time-resolved photoemission electron microscopy setup. The experiments are supported by finite-difference time-domain simulations of similar silver structures. The observed differences in the field dynamics across a single particle do not reflect differences in plasmon resonance frequency or dephasing time. They instead arise from a combination of retardation effects and the coherent superposition between multiple plasmon modes of the particle, inherent to a few-cycle pulse excitation. The ability to detect and predict local variations in the few-femtosecond time evolution of multimode coherent plasmon excitations in rationally synthesized nanoparticles can be used in the tailoring of nanostructures for ultrafast and nonlinear plasmonics.

We measure spectrally and spatially resolved high-order harmonics generated in argon using chirped multi-cycle laser pulses. Using a stable, high-repetition rate laser we observe detailed interference structures in the far-field. The structures are of two kinds; off-axis interference from the long trajectory only and on-axis interference including the short and long trajectories. The former is readily visible in the far-field spectrum, modulating both the spectral and spatial profile. To access the latter, we vary the chirp of the fundamental, imparting different phases on the different trajectories, thereby changing their relative phase. Using this method together with an analytical model, we are able to explain the on-axis behaviour and access the dipole phase parameters for the short (a s ) and long (a l ) trajectories. The extracted results compare very well with phase parameters calculated by solving the time-dependent Schrödinger equation. Going beyond the analytical model, we are also able to successfully reproduce the off-axis interference structure.

Abstract. We study high-order harmonic generation with a high-repetition rate (200 kHz), few-cycle, driving laser, based on optical parametric chirped pulse amplification. The system delivers carrier-envelope phase stable, 8 fs, 10 μJ pulses at a central wavelength of 890 nm. High-order harmonics, generated in a high-pressure Ar gas jet, exhibit a strong CEP-dependence over a large spectral range owing to excellent stability of the driving laser pulses. This range can be divided into three spectral regions with distinct CEP influence. The observed spectral interference structures are explained by an analytical model based upon multiple pulse interferences.

We generate high-order harmonics at high pulse repetition rates using a turnkey laser. High-order harmonics at 400 kHz are observed when argon is used as target gas. In neon, we achieve generation of photons with energies exceeding 90 eV (∼13 nm) at 20 kHz. We measure a photon flux of up to 4.4 × 10(10) photons per second per harmonic in argon at 100 kHz. Many experiments employing high-order harmonics would benefit from higher repetition rates, and the user-friendly operation opens up for applications of coherent extreme ultra-violet pulses in new research areas.

We demonstrate control of near-field localization within individual silver nanocubes through photoemission electron microscopy combined with broadband, few-cycle laser pulses. We find that the near-field is concentrated at the corners of the cubes, and that it can be efficiently localized to different individual corners depending on the polarization of the incoming light. The experimental results are confirmed by finitedifference time-domain simulations, which also provide an intuitive picture of polarization dependent near-field localization in nanocubes.

The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-cycle change of the initial velocity distribution of the electron and its excursion time. The resonant enhancement is observed only for the long trajectory contribution of a particular harmonic when a window resonance in argon, which is off-resonant in the field-free case, is shifted into resonance due to a large dynamic Stark shift.

The direct detection of the spatiotemporal dynamics of nanolocalized optical near-fields on nanostructured metal surfaces, for example, imaging of localized surface plasmons (cf. Chapter 1) on rough or nanostructured metal films or the imaging of propagating surface plasmon polaritons at a vacuum-metal or metal-dielectric interface is a prerequisite to further control and optimize surface-plasmon based ultrafast nanooptics for future device development and applications [1][2][3][4].While free electrons in metals collectively respond to excitation from a light pulse, which is resonant to the surface plasmon frequency of the system, and squeeze and amplify the field intensity of the incoming plane light field into a subwavelength spatial volume, the typically broad frequency bandwidth of surface plasmon resonances supports an ultrafast response of these fields with rapid field changes on sub-femtosecond time scales [5].The sub-wavelength nanoscaled localization of optical fields in the vicinity of metal nanostructures and the ultrafast temporal evolution of such fields on a 0.1-100 fs time scale require the invention and development of new experimental methodologies, which combine nanometer (sub-optical) spatial resolution, sub-femtosecond temporal resolution, and optionally further nanospectroscopic information.Resolving the spatial distribution of such fields requires a microscopic technique with sub-optical spatial resolution, for example, in the 10-100 nm range. Scanning near-field optical microscopy (SNOM) techniques have been successfully applied with spatial resolutions of about ∼100 nm; however, the combination with ultrashort light pulses is still very difficult. Photoemission electron microscopy (PEEM) is a technique capable of resolving the spatial emission distribution of photoelectrons with an ultimate resolution of ∼10 nm.

Surface electron dynamics unfold at time and length scales down to attoseconds and nanometres, making direct imaging with extreme spatiotemporal resolution highly desirable. However, this has turned out to be a major challenge even with the advent of reliable attosecond light sources. In this paper, photoelectrons from Ag nanowires and nanoparticles excited by extreme ultraviolet (XUV) attosecond pulse trains and infrared femtosecond pulses using a PhotoEmission Electron Microscope (PEEM) are imaged. In addition, the samples were investigated using Scanning Electron Microscopy (SEM) and synchrotron based X-ray photoelectron spectroscopy (XPS). To achieve contrast between the nanostructures and the substrate in the XUV images, three different substrate materials were investigated: Cr, ITO and Au. While plasmonic field enhancement can be observed on all three substrates, only on Au substrates do the Ag nanowires appear significantly brighter than the substrate in XUV-PEEM imaging. 3-photon photoemission imaging of plasmonic hot-spots was performed where the autocorrelation trace is observed in the interference signal between two femtosecond Infra-Red (IR) beams with sub-cycle precision. Finally, using Monte Carlo simulations, it is shown how the secondary electrons imaged in the XUV PEEM can potentially reveal information on the attosecond time scale from the near surface region of the nanostructures.