Delocalization of Nonlinear Optical Responses in Plasmonic Nanoantennas
Remote excitation and emission of two-photon luminescence and second-harmonic generation are observed in micrometer long gold rod optical antennas upon local illumination with a tightly focused near-infrared femtosecond laser beam. We show that the nonlinear radiations can be emitted from the entire antenna and the measured far-field angular patterns bear the information regarding the nature and origins of the respective nonlinear processes. We demonstrate that the nonlinear responses are transported by the propagating surface plasmon at excitation frequency, enabling thereby polariton-mediated tailoring and design of nonlinear responses.
A size dependent discontinuous decay rate for the exciton emission in ZnO quantum dots
The time resolved UV-fluorescence in ZnO quantum dots has been investigated using femtosecond laser spectroscopy. The measurements were performed as a function of particle size for particles between 3 and 7 nm in diameter, which are in the quantum confined regime. A red shift in the fluorescence maximum is seen while increasing the particle size, which correlates with the shift in band gap due to quantum confinement. The energy difference between the UV-fluorescence and the band gap does, however, increase for the smaller particles. For 3.7 nm particles the fluorescence energy is 100 meV smaller than the band gap energy, whereas it is only 20 meV smaller for the largest particles. This indi…
Scanning optical microscopy modeling in nanoplasmonics
International audience; One of the main purposes of nanoplasmonics is the miniaturization of optical and electro-optical components that could be integrable in coplanar geometry. In this context, we propose a numerical model of a polarized scanning optical microscope able to faithfully reproduce both photon luminescence and temperature distribution images associated with complex plasmonic structures. The images are computed, pixel by pixel, through a complete self-consistent scheme based on the Green dyadic functions (GDF) formalism. The basic principle consists in the numerical implementation of a realistic three-dimensional light beam acting as a virtual light tip able to probe the volume…
Electrostatic Control over Optically Pumped Hot Electrons in Optical Gap Antennas
International audience; We investigate the influence of a static electric field on the incoherent nonlinear response of an unloaded electrically contacted nanoscale optical gap antenna. Upon excitation by a tightly focused near-infrared femtosecond laser beam, a transient elevated temperature of the electronic distribution results in a broadband emission of nonlinear photoluminescence (N-PL). We demonstrate a modulation of the yield at which driving photons are frequency up-converted by means of an external control of the electronic surface charge density. We show that the electron temperature and consequently the N-PL intensity can be enhanced or reduced depending on the command polarity a…
Hot electrons and nonlinear optical nanoantennas
The large field enhancement generated at the surface of a resonant plasmonic nanoparticle, or optical antennas, is the key mechanism that eventually led to the development of nonlinear plasmonics [1-2]. While the resonance may boost the nonlinear yield of an adjacent structure or surrounding medium, it was soon realized that optical antennas possess nonlinear coefficients comparable or exceeding those of standard nonlinear optical materials [3]. We discuss here two nonlinear optical processes — incoherent multi-photon luminescence (MPL) and coherent second-harmonic generation (SHG) — emitted from gold rod optical antennas upon local illumination with a tightly focused femtosecond near-infra…
Spatial Distribution of the Nonlinear Photoluminescence in Au Nanowires
When gold nanowires are excited with a tightly focused femtosecond laser a distributed nonlinear photoluminescence (N-PL) develops throughout the entire structure. A complete spaced-resolved analysis of the spectral signature of the nanowire nonlinear response is carried out to understand the origin of the distributed nonlinear response. We discuss various mechanisms to explain the experimental data and unambiguously demonstrate that the spatial and spectral extension of the N-PL in the nanowire are mainly dictated by the propagation of a surface plasmon excited at the pump wavelength. We also present experimental signature of near-field excitation of a broadband continuum of surface plasmo…