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The excitation of nanoscale near-fields with ultrashort and intense laser pulses of well-defined waveform enables strongly spatially and temporally localized electron emission, opening up the possibility for the generation of attosecond electron pulses. Here, we investigate the electron photoemission from isolated nanoparticles of different materials in few-cycle laser fields at intensities where the Coulomb field of the ionized electrons and residual ions significantly contribute to the electron acceleration process. The dependences of the electron cut-off energy on the material’s dielectric properties and electron binding energy are investigated systematically in both experiments and semi-classical simulations. We find that for sufficiently high near-field intensities the material dependence of the acceleration in the enhanced near-fields is quenched by many-particle charge-interaction.

Field localization by nanostructures illuminated with laser pulses of well-defined waveform enables spatio-temporal tailoring of the near-fields for sub-cycle control of electron dynamics at the nanoscale. Here, we apply intense linearly-polarized two-color laser pulses for all-optical control of the highest energy electron emission from SiO2 nanoparticles. For the size regime where light propagation effects become important, we demonstrate the possibility to control the preferential emission angle of a considerable fraction of the fastest electrons by varying the relative phase of the two-color field. Trajectory based semi-classical simulations show that for the investigated nanoparticle size range the directional steering can be attributed to the two-color effect on the electron trajectories, while the accompanied modification of the spatial distribution of the ionization rate on the nanoparticle surface has only a minor effect.

The diversity of nanoparticle shapes generated by condensation from gaseous matter reflects the fundamental competition between thermodynamic equilibration and the persistence of metastable configurations during growth. In the kinetically limited regime, intermediate geometries that are favoured only in early formation stages can be imprinted in the finally observed ensemble of differently structured specimens. Here we demonstrate that single-shot wide-angle scattering of femtosecond soft X-ray free-electron laser pulses allows three-dimensional characterization of the resulting metastable nanoparticle structures. For individual free silver particles, which can be considered frozen in space for the duration of photon exposure, both shape and orientation are uncovered from measured scattering images. We identify regular shapes, including species with fivefold symmetry and surprisingly large aspect ratio up to particle radii of the order of 100 nm. Our approach includes scattering effects beyond Born’s approximation and is remarkably efficient—opening up new routes in ultrafast nanophysics and free-electron laser science., Nature Communications, 6 (1), ISSN:2041-1723