Variable-angle and Mueller matrix spectroscopic ellipsometry are used to determine the effective dielectric tensors of random and aligned silver nanoparticles and nanorods thin films. Randomly arranged particles are uniaxially anisotropic while aligned particles are biaxially anisotropic, with the anisotropy predominantly at the plasmonic resonances. The strong resonances in nanorod arrays result in the real part of the effective in-plane permittivities being opposite in sign over a significant range in the visible, suggesting the potential to design materials that display tunable negative-refraction. A structural tilt in the particle arrays results in monoclinic dielectric properties.
We present highly ordered Ag nanowire arrays with 35nm periodicity grown on patterned templates. The optical properties measured using generalized ellipsometry exhibit strong anisotropy. Dielectric functions are calculated by fitting the Jones matrix elements with a biaxial layer model, accounting for both metallic behavior and localized surface plasmon resonances. The amplitude and wavelength maximum of the plasmon resonance perpendicular to the wires increase with increasing wire width and thickness. The dielectric coefficients of 10-mm-wide nanowires show a transition behavior from insulating in UV to metallic above 550nm. Their potential application as polarization-dependent plasmonic-scattering transparent conductive electrodes is discussed.
Silver nanoparticles and nanowires self-aligned on pre-patterned rippled substrate are presented as active surface enhanced Raman scattering (SERS) substrates. The reported inter-particle gap of 5 nm and array periodicity of 35 nm are much lower than current lithographic limits. The observed anisotropy in SERS and surface plasmon resonance in such arrays is attributed to different plasmonic field enhancement along and across the chains of nanoparticles not due to shape anisotropy. For nanoparticle arrays higher SERS intensity is found along the particle chain, but for nanowire arrays higher SERS intensity is found for excitation across the wires. Higher intensity across nanowire arrays supports the argument that the SERS phenomenon is due to electromagnetic field enhancement (hot-junctions) caused by localized surface plasmon resonance across the nanowires having a 35 nm gap. The effect of inter-particle gap, ordering, and aspect ratio on field enhancement is demonstrated. Higher SERS intensity is observed in aligned elongated nanoparticles compared to aligned spherical, non-ordered nanoparticles, or aligned nanowires. Aligned silver nanowires enhance Raman scattering more strongly than aligned gold nanowires.
Highly ordered Ag nanocluster structures have been grown on pre-patterned amorphous SiO(2) surfaces by oblique angle physical vapor deposition at room temperature. Despite the small undulation of the rippled surface, the stripe-like Ag nanoclusters are very pronounced, reproducible and well separated. Computer modeling of the growth has been performed with a lattice-based kinetic Monte Carlo (KMC) method using a combination of a simplified inter-atomic potential and experimental transition barriers taken from the literature. An effective transition event classification method is introduced which allows a boost factor of several thousand compared to a traditional KMC approach, thus allowing experimental time scales to be modeled. The simulation predicts a low sticking probability for the arriving atoms, millisecond order lifetimes for single Ag adatoms and ≈1 nm square surface migration ranges of Ag adatoms. It is also shown that metal nucleations can trigger even on defect free surfaces. The simulations give excellent reproduction of the experimentally observed nanocluster growth patterns.
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