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Metasurfaces, and in particular those containing plasmonic-based metallic elements, constitute a particularly attractive set of materials. By means of modern nanolithographic fabrication techniques, flat, ultrathin optical elements may be constructed . However, in spite of their strong optical nonlinearities, plasmonic metasurfaces have so far been investigated mostly in the linear regime. Here we introduce full nonlinear phase control over plasmonic elements in metasurfaces. We show that for nonlinear interactions in a phase-gradient nonlinear metasurface a new anomalous nonlinear phase matching condition prevails, which is the nonlinear analog of the generalized Snell law demonstrated for linear metasurfaces. This phase matching condition is very different from the other known phase matching schemes. The subwavelength phase control of optical nonlinearities provides a foundation for the design of flat nonlinear optical elements based on metasurfaces. Our demonstrated flat nonlinear elements (i.e. lenses) act as generators and manipulators of the frequency-converted signal.
Optimizing the shape of nanostructures and nano antennas for specific optical properties has evolved to be a very fruitful activity. With modern fabrication tools a large variety of possibilities is available for shaping both nanoparticles and nanoca vities; in particular nanocavities in thin metal films have emerged as attractive candidates for new metamaterials and strong linear and nonlinear optical systems. Here we rationally design metallic nanocavities to boost their Four Wave Mixing response by resonating the optical plasmonic resonances with the incoming and generated beams. The linear and nonlinear optical responses as well as the propagation of the electric fields inside the cavities are derived from the solution of Maxwell equations by using the 3D finite-differences time domain method. The observed conversion-efficiency of near infra-red to visible light equals or surpasses that of BBO of equivalent thickness. Implications to further optimization for efficient and broadband ultrathin nonlinear optical materials are discussed.
When two or more metallic nanoparticles are in close proximity, their plasmonic modes may interact through the near field, leading to additional resonances of the coupled system or to shifts of their resonant frequencies. This process is analogous to atom-hybridization, as had been proposed by Gersten and Nitzan and modeled by Nordlander et al. The coupling between plasmonic modes can be in-phase (symmetric) or out-of-phase (anti-symmetric), reflecting correspondingly, the bonding and anti-bonding nature of such configurations. Since the incoming light redistributes the charge distribution around the metallic nanoparticles, its polarization features play a major role in the nonlinear optical probing of the energy-level landscape upon hybridization. Thus, controlling the nature of coupling between metallic nanostructures is of a great importance as it enables tuning their spectral responses leading to novel devices which may surpass the diffraction limit.
We demonstrate noncontact, high quality surface modification with spatial resolution of ~20 nm. The nanowriting is based on the interaction between the surface and the tip of an Atomic force microscope illuminated by a focused laser beam and hovering 1-4 nanometers above the surface without touching it. The floating tip nanowriting is compared to mechanical surface scratching, and is found to be much more reproducible, and of higher quality. In an Apertureless Scanning Near Field Optical Microscope geometry the tip is illuminated by a focused femtosecond laser, leading to two different, clearly identifiable mechanisms for removing material from the surface: when heated by the laser beam, the hot-tip thermally patterns the surface of low melting temperature soft materials, and when focused right at the apex of the sharp tip, the enhanced electric field of the laser beam causes ablation in high melting temperature metal films.
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