René Kullock

Polarization conversion through collective surface plasmons in metallic nanorod arrays

For two-dimensional (2D) arrays of metallic nanorods arranged perpendicular to a substrate several methods have been proposed to determine the electromagnetic near-field distribution and the surface plasmon resonances, but an analytical approach to explain all optical features on the nanometer length scale has been missing to date. To fill this gap, we demonstrate here that the field distribution in such arrays can be understood on the basis of surface plasmon polaritons (SPPs) that propagate along the nanorods and form standing waves. Notably, SPPs couple laterally through their optical near fields, giving rise to collective surface plasmon (CSP) effects. Using the dispersion relation of such CSPs, we deduce the condition of standing-wave formation, which enables us to successfully predict several features, such as eigenmodes and resonances. As one such property and potential application, we show both theoretically and in an experiment that CSP propagation allows for polarization conversion and optical filtering in 2D nanorod arrays. Hence, these arrays are promising candidates for manipulating the light polarization on the nanometer length scale.

Metallic nanorod arrays: negative refraction and optical properties explained by retarded dipolar interactions

We show that the optical properties of arrays of parallel-aligned metallic nanorods can be understood by means of a retarded dipolar interaction model. Exemplarily, arrays of gold nanorods having various lengths and diameters are investigated experimentally. A strong diameter dependence of the long-axis surface plasmon resonance (LSPR) as well as a lower energy limit of this mode for varying length was found. The model also shows that, for small nanorod distances (d<λ/2), the optical properties are independent of the azimuthal angle of the incoming plane wave and of the detailed arrangement of the nanorods. Furthermore, the model was used to explain the dependence of the LSPR on the angle of incidence and to find the conditions for which negative and extraordinary positive refractions occur in these structures.

SHG simulations of plasmonic nanoparticles using curved elements

We demonstrate that simulating plasmonic nanostructures by means of curved elements (CEs) significantly increases the accuracy and computation speed not only in the linear but also in the nonlinear regime. We implemented CEs within the discontinuous Galerkin (DG) method and, as an example of a nonlinear effect, investigated second-harmonic generation (SHG) at a silver nanoparticle. The second-harmonic response of the material is simulated by an extended Lorentz model (ELM). In the linear regime the CEs are ≈ 9 times faster than ordinary elements for the same accuracy, provide a much better convergence and show fewer unphysical field artifacts. For DG-SHG calculations CEs are almost indispensable to obtain physically reasonable results at all. Additionally, their boundary approximation has to be of the same order as their polynomial degree to achieve artifact-free field distributions. In return, the use of such CEs with the DG method pays off more than evidently, since the additional computation time is only 1%.

Three-dimensional, arbitrary orientation of focal polarization

We demonstrate a simple setup for generating a three-dimensional arbitrary orientation of the polarization vector in a laser focus. The key component is the superposition of a linearly and a radially polarized laser beam, which both can be controlled individually in intensity and relative phase. We exemplify the usefulness of this setup by determining the spatial orientation of a single silver nanorod in three-dimensional space by recording the angle-variable backscattered light intensity.

Local photochemical plasmon mode tuning in metal nanoparticle arrays

We report on the local modification of gold nanoparticle arrays by photochemical deposition of gold from solution. Our method allows to alter the localized surface plasmon resonance (LSPR) in a restricted area by exposure of gold salt (HAuCl4) to light, whereas the expansion of such sections depends on the illumination optics. The geometry parameters of the individual nanoparticles in the modified regions are characterized by SEM and AFM, while the optical properties of distinct array sections are analyzed by means of optical spectroscopy. A blueshift of the surface plasmon resonance wavelength is observed upon the deposition process. An explanation for the blueshift is found by performing calculations using an analytical dipolar interaction model (DIM), which allows us to distinguish the individual contributions of the particle geometry on the one hand and the changes in particle interaction on the other hand. The resulting simulated scattering spectra verify the blueshift of the LSPR, which can be attributed to an increase in aspect ratio of the particles during growth. Since plasmonically active nanoparticle arrays are known to be candidates for sensing applications, this method and the gained understanding can be exploited to fabricate large sensor substrates with local LSPR variations.