An unambiguous determination of the three-dimensional structure of nanoparticles is challenging. Electron tomography requires a series of images taken for many different specimen orientations. This approach is ideal for stable and stationary structures. But ultrasmall nanoparticles are intrinsically structurally unstable and may interact with the incident electron beam, constraining the electron beam density that can be used and the duration of the observation. Here we use aberration-corrected scanning transmission electron microscopy, coupled with simple imaging simulation, to determine with atomic resolution the size, three-dimensional shape, orientation and atomic arrangement of size-selected gold nanoclusters that are preformed in the gas phase and soft-landed on an amorphous carbon substrate. The structures of gold nanoclusters containing 3096 atoms can be identified with either Ino-decahedral, cuboctahedral or icosahedral geometries. Comparison with theoretical modelling of the system suggests that the structures are consistent with energetic considerations. The discovery that nanoscale gold particles function as active and selective catalysts for a variety of important chemical reactions has provoked much research interest in recent years. We believe that the detailed structure information we provide will help to unravel the role of these nanoclusters in size- and structure-specific catalytic reactions. We note that the technique will be of use in investigations of other supported ultrasmall metal cluster systems.
We demonstrate nonlinear excitation of surface plasmons on a gold film by optical four-wave mixing. Two excitation beams of frequencies omega(1) and omega(2) are used in a modified Kretschmann configuration to induce a nonlinear polarization at a frequency of omega(4wm)=2omega(1)-omega(2), which gives rise to surface plasmon excitation at a frequency of omega(4wm). We observe a characteristic plasmon dip at the Kretschmann angle and explain its origin in terms of destructive interference. Despite a nonvanishing bulk response, surface plasmon excitation by four-wave mixing is dominated by a nonlinear surface polarization. To interpret and validate our results, we provide a comparison with second-harmonic generation.
Plasmonics is considered as one of the most promising candidates for implementing the next generation of ultrafast and ultracompact photonic circuits. Considerable effort has been made to scale down individual plasmonic components into the nanometer regime. However, a compact plasmonic source that can efficiently generate surface plasmon polaritons (SPPs) and deliver SPPs to the region of interest is yet to be realized. Here, bridging the optical antenna theory and the recently developed concept of metamaterials, we demonstrate a subwavelength, highly efficient plasmonic source for directional generation of SPPs. The designed device consists of two nanomagnetic resonators with detuned resonant frequencies. At the operating wavelength, incident photons can be efficiently channeled into SPP waves modulated by the electric field polarization. By tailoring the relative phase at resonance and the separation between the two nanoresonators, SPPs can be steered to predominantly propagate along one specific direction. This novel magnetic nanoantenna paves a new way to manipulate photons in the near-field, and also could be useful for SPP-based nonlinear applications, active modulations, and wireless optical communications.
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