Ultrafast Coupling of Optical Near Fields to Low-Energy Electrons Probed in a Point-Projection Microscope.

We report the first observation of the coupling of strong optical near fields to wavepackets of free, 100 eV electrons with <50 fs temporal resolution in an ultrafast point-projection microscope. Optical near fields are created by excitation of a thin, nanometer-sized Yagi-Uda antenna, with 20 fs near-infrared laser pulses. Phase matching between electrons and near fields is achieved due to strong spatial confinement of the antenna near field. Energy-resolved projection images of the antenna are recorded in an optical pump-electron probe scheme. We show that the phase modulation of the electron by transverse-field components results in a transient electron deflection while longitudinal near-field components broaden the kinetic energy distribution. This low-energy electron near-field coupling is used here to characterize the chirp of the ultrafast electron wavepackets, acquired upon propagation from the electron emitter to the sample. Our results bring direct mapping of different vectorial components of highly localized optical near fields into reach.

Observing charge separation in nanoantennas via ultrafast point-projection electron microscopy.

Observing the motion of electrons on their natural nanometer length and femtosecond time scales is a fundamental goal of and an open challenge for contemporary ultrafast science1-5. At present, optical techniques and electron microscopy mostly provide either ultrahigh temporal or spatial resolution, and microscopy techniques with combined space-time resolution require further development6-11. In this study, we create an ultrafast electron source via plasmon nanofocusing on a sharp gold taper and implement this source in an ultrafast point-projection electron microscope. This source is used in an optical pump-electron probe experiment to study ultrafast photoemissions from a nanometer-sized plasmonic antenna12-15. We probe the real space motion of the photoemitted electrons with a 20-nm spatial resolution and a 25-fs time resolution and reveal the deflection of probe electrons by residual holes in the metal. This is a step toward time-resolved microscopy of electronic motion in nanostructures.

Long-lived electron emission reveals localized plasmon modes in disordered nanosponge antennas.

We report long-lived, highly spatially localized plasmon states on the surface of nanoporous gold nanoparticles-nanosponges-with high excitation efficiency. It is well known that disorder on the nanometer scale, particularly in two-dimensional systems, can lead to plasmon localization and large field enhancements, which can, in turn, be used to enhance nonlinear optical effects and to study and exploit quantum optical processes. Here, we introduce promising, three-dimensional model systems for light capture and plasmon localization as gold nanosponges that are formed by the dewetting of gold/silver bilayers and dealloying. We study light-induced electron emission from single nanosponges, a nonlinear process with exponents of n≈5...7, using ultrashort laser pulse excitation to achieve femtosecond time resolution. The long-lived electron emission process proves, in combination with optical extinction measurements and finite-difference time-domain calculations, the existence of localized modes with lifetimes of more than 20 fs. These electrons couple efficiently to the dipole antenna mode of each individual nanosponge, which in turn couples to the far-field. Thus, individual gold nanosponges are cheap and robust disordered nanoantennas with strong local resonances, and an ensemble of nanosponges constitutes a meta material with a strong polarization independent, nonlinear response over a wide frequency range.