Matthew D. Arnold

A review of the optical properties of alloys and intermetallics for plasmonics

Alternative materials are required to enhance the efficacy of plasmonic devices. We discuss the optical properties of a number of alloys, doped metals, intermetallics, silicides, metallic glasses and high pressure materials. We conclude that due to the probability of low frequency interband transitions, materials with partially occupied d states perform poorly as plasmonic materials, ruling out many alloys, intermetallics and silicides as viable. The increased probability of electron-electron and electron-phonon scattering rules out many doped and glassy metals.

Plasmonic Resonances of Closely Coupled Gold Nanosphere Chains

The optical properties of an ordered array of gold nanospheres have been calculated using the T-matrix method in the regime where the near-fields of the particles are strongly coupled. The array consists of a one-dimensional chain of spheres of 15 nm diameter where the number of spheres in the chain and interparticle spacing is varied. Calculations have been performed with chains up to 150 particles in length and with an interparticle spacing between 0.5 and 30 nm. Incident light polarized along the axis of the chain (longitudinal) and perpendicular (transverse) to it are considered, and in the latter case for wavevectors along and perpendicular to the chain axis. For fixed chain length the longitudinal plasmon resonance red shifts, relative to the resonance of an isolated sphere, as the interparticle spacing is reduced. The shift in the plasmon resonance does not appear to follow an exponential dependence upon gap size for these extended arrays of particles. The peak shift is inversely proportional to th...

Chiral mirror and optical resonator designs for circularly polarized light: suppression of cross-polarized reflectances and transmittances

Abstract A left-handed chiral sculptured thin film (STF) that reflects strongly at the wavelength of the circular Bragg resonance tends to partially convert the handedness of incident LCP (left-circularly-polarized) light to RCP (right-circularly-polarized). We show that the cross-polarized component of the reflected RCP beam can be eliminated by interference with an additional RCP beam that is reflected at the interface of an isotropic cover and an AR (antireflecting) layer. For best results the refractive index and thickness of the AR layer need to accommodate a phase change on reflection that occurs at the chiral film. Effective suppression of the reflectances RRR, RRL, RLR and the transmittances TRL, TLR can be achieved by sandwiching the chiral reflector between such amplitude and phase-matched AR coatings. Co-polarized chiral reflectors of this type may form efficient handed optical resonators. For LCP light the optical properties of such a handed resonator are formally the same as the properties of the isotropic passive or active Fabry–Perot resonators, but the handed resonator is transparent to RCP light.

Natural and Nanoengineered Chiral Reflectors: Structural Color of Manuka Beetles and Titania Coatings

A parallel study of natural and nanoengineered structurally chiral reflecting coatings is described. It is shown that the nanostructures are different in a minor way but are optically equivalent. Refractive index matching of nanoengineered chiral coatings on a plane substrate is shown to improve the saturation of structural color. Optical and electron microscopies reveal complexity in the multilayered chiral coatings that produce green metallic-like reflections from manuka (scarab) beetles. In particular, the reflectors are shown to have the form of small concave pits and troughs that are filled with contouring chiral material. Each chiral microreflector presents a range of pitch and tilt to an incident beam of light. Physical properties of the textured coatings are related to optical properties such as spectral reflectance, angle of spread, and perceived color, which has a high degree of saturation due to the filling of the pits. Observations of overlapping chiral mediums in beetle reflectors have inspired nanoengineering of related handed media such as Bragg reflectors for elliptically polarized light.

Designing materials for plasmonic systems: the alkali-noble intermetallics

We use electronic structure calculations based upon density functional theory to search for ideal plasmonic materials among the alkali-noble intermetallics. Importantly, we use density functional perturbation theory to calculate the electron-phonon interaction and from there use a first order solution to the Boltzmann equation to estimate the phenomenological damping frequency in the Drude dielectric function. We discuss the necessary electronic features of a plasmonic material and investigate the optical properties of the alkali-noble intermetallics in terms of some generic plasmonic system quality factors. We conclude that at low negative permittivities, KAu, with a damping frequency of 0.0224 eV and a high optical gap to bare plasma frequency ratio, outperforms gold and to some extent silver as a plasmonic material. Unfortunately, a low plasma frequency (1.54 eV) reduces its utility in modern plasmonics applications. We also discuss, briefly, the effect of local fields on the optical properties of these materials.

Li-ion adsorption and diffusion on two-dimensional silicon with defects: a first principles study.

Using first principles calculations we investigate the binding and diffusion of Li on silicene and evaluate the prospects for application to Li-ion batteries. We find that the defect formation energy for silicene is half that of graphene, showing that silicene is more likely to contain defects. The overall lithium adsorption energy on silicene with defects is greater than the bulk cohesive energy of lithium giving stability for use in storage. Our results predict high mobility for lithium atoms on the surface of silicene with energy barriers in the range of 0.28-0.30 eV. Further, we find that the diffusion barrier through silicene is significantly lower than the diffusion barrier through graphene, with a value of 0.05 eV for the double vacancy and 0.88 eV for the single vacancy. The low diffusion barriers, both on the surface and through the hollow site, suggest a suitable material for use in Li-ion batteries.

An Efficient Solution for Scattering by a Perfectly Conducting Strip Grating

An efficient implementation of a Wiener-Hopf solution for complementary strip gratings is presented. Acceleration of the required infinite product is achieved via a hybrid approach involving a gamma function expression for the infinite product of Taylor approximated terms. The efficiency of the accelerated method is compared to the brute-force method as a function of system parameters.

Optical properties of intermetallic compounds from first principles calculations: a search for the ideal plasmonic material

First principles calculations have been used to predict the optical properties for a range of intermetallic compounds for which little or no experimental optical data are currently available. Density functional theory combined with the random phase approximation is used to calculate the dielectric functions for these compounds. The aim of this work is to investigate how the band edge and plasma frequency vary with composition in order to identify materials with promising plasmonic properties. Towards this end the intermetallic compounds chosen are composed of elements which on their own have reasonable optical properties for plasmonic applications. The position of the band edge relative to the plasma frequency is most favourable in the simple binary compounds formed from the alkali plus noble metals NaAu, KAu and KAg. In particular, for KAu the band edge and plasma frequency occur at almost the same frequency, and hence the imaginary part of the dielectric function is practically zero for frequencies below the plasma frequency. In addition, the plasma frequency in this compound is at relatively low frequency, promising a material with strong plasmon response in the infrared.

Transmitting hertzian optical nanoantenna with free-electron feed.

A pair of coupled gold nanorods excited by a beam of free electrons acts as a transmitting Hertzian antenna in the optical part of the spectrum. Significantly enhanced resonant emission is observed from the antenna when the electron beam is injected around the junction between the rods, where the local density of electromagnetic states is elevated.

An improved transfer-matrix model for optical superlenses.

The use of transfer-matrix analyses for characterizing planar optical superlensing systems is studied here, and the simple model of the planar superlens as an isolated imaging element is shown to be defective in certain situations. These defects arise due to neglected interactions between the superlens and the spatially varying shadow masks that are normally used as scattering objects for imaging, and which are held in near-field proximity to the superlenses. An extended model is proposed that improves the accuracy of the transfer-matrix analysis, without adding significant complexity, by approximating the reflections from the shadow mask by those from a uniform metal layer. Results obtained using both forms of the transfer matrix model are compared to finite element models and two example superlenses, one with a silver monolayer and the other with three silver sublayers, are characterized. The modified transfer matrix model gives much better agreement in both cases.