ABSTRACT
Interactions between plasmons and exciton nanoemitters in plexcitonic systems lead to fast and intense luminescence, desirable in optoelectonic devices, ultrafast optical switches and quantum information science. While luminescence enhancement through exciton-plasmon coupling has thus far been mostly demonstrated in micro- and nanoscale structures, analogous demonstrations in bulk materials have been largely neglected. Here we present a bulk nanocomposite glass doped with cadmium telluride quantum dots (CdTe QDs) and silver nanoparticles, nAg, which act as exciton and plasmon sources, respectively. This glass exhibits ultranarrow, FWHM = 13 nm, and ultrafast, 90 ps, amplified photoluminescence (PL), λemâ 503 nm, at room temperature under continuous-wave excitation, λexc = 405 nm. Numerical simulations confirm that the observed improvement in emission is a result of a multiscale light enhancement owing to the ensemble of QD-populated plasmonic nanocavities in the material. Power-dependent measurements indicate that >100 mW coherent light amplification occurs. These types of bulk plasmon-exciton composites could be designed comprising a plethora of components/functionalities, including emitters (QDs, rare earth and transition metal ions) and nanoplasmonic elements (Ag/Au/TCO, spherical/anisotropic/miscellaneous), to achieve targeted applications.
ABSTRACT
Zinc oxide-zinc tungstate (ZnO-ZnWO4 ) is a self-organized eutectic composite consisting of parallel ZnO thin layers (lamellae) embedded in a dielectric ZnWO4 matrix. The electromagnetic behavior of composite materials is affected not only by the properties of single constituent materials but also by their reciprocal geometrical micro-/nano-structurization, as in the case of ZnO-ZnWO4 . The light interacting with microscopic structural features in the composite material provides new optical properties, which overcome the possibilities offered by the constituent materials. Here remarkable active and passive polarization control of this composite over various wavelength ranges are shown; these properties are based on the crystal orientation of ZnO with respect to the biaxiality of the ZnWO4 matrix. In the visible range, polarization-dependent polarized luminescence occurs for blue light emitted by ZnO. Moreover, it is reported on the enhancement of the second harmonic generation of the composite with respect to its constituents, due to the phase matching condition. Finally, in the medium infrared spectral region, the composite behaves as a metamaterial with strong polarization dependence.
ABSTRACT
Second-order nonlinear optical materials are used to generate new frequencies by exploiting second-harmonic generation (SHG), a phenomenon where a nonlinear material generates light at double the optical frequency of the input beam. Maximum SHG is achieved when the pump and the generated waves are in phase, for example through birefringence in uniaxial crystals. However, applying these materials usually requires a complicated cutting procedure to yield a crystal with a particular orientation. Here we demonstrate the first example of phase matching under the normal incidence of SHG in a biaxial monoclinic single crystal of zinc tungstate. The crystal was grown by the micro-pulling-down method with the (102) plane perpendicular to the growth direction. Additionally, at the same time white light was generated as a result of stimulated Raman scattering and multiphoton luminescence induced by higher-order effects such as three-photon luminescence enhanced by cascaded third-harmonic generation. The annealed crystal offers SHG intensities approximately four times larger than the as grown one; optimized growth and annealing conditions may lead to much higher SHG intensities.
