Debabrata Sikdar

Tunable terahertz left-handed metamaterial based on multi-layer graphene-dielectric composite

A terahertz fishnet metamaterial, consisting of a gallium arsenide substrate sandwiched between multi-layer graphene-dielectric composites, is theoretically studied. Detailed analysis shows that this metamaterial has a left-handed transmission peak accompanied with an abnormal phase dispersion and a clear negative refractive index which originates from simultaneous magnetic and electric resonances. Our structure is unique because it has no metallic parts to achieve the left-handed properties. The most important utility of this metamaterial comes from the fact that its left-handed features can be dynamically controlled by applying external bias to shift the Fermi level in graphene.

Optically resonant magneto-electric cubic nanoantennas for ultra-directional light scattering

Cubic dielectric nanoparticles are promising candidates for futuristic low-loss, ultra-compact, nanophotonic applications owing to their larger optical coefficients, greater packing density, and relative ease of fabrication as compared to spherical nanoparticles; besides possessing negligible heating at nanoscale in contrast to their metallic counterparts. Here, we present the first theoretical demonstration of azimuthally symmetric, ultra-directional Kerkers-type scattering of simple dielectric nanocubes in visible and near-infrared regions via simultaneous excitation and interference of optically induced electric- and magnetic-resonances up to quadrupolar modes. Unidirectional forward-scattering by individual nanocubes is observed at the first generalized-Kerkers condition for backward-scattering suppression, having equal electric- and magnetic-dipolar responses. Both directionality and magnitude of these unidirectional-scattering patterns get enhanced where matching electric- and magnetic-quadrupolar responses spectrally overlap. While preserving azimuthal-symmetry and backscattering suppression, a nanocube homodimer provides further directionality improvement for increasing interparticle gap, but with reduced main-lobe magnitude due to emergence of side-scattering lobes from diffraction-grating effect. We thoroughly investigate the influence of interparticle gap on scattering patterns and propose optimal range of gap for minimizing side-scattering lobes. Besides suppressing undesired side-lobes, significant enhancement in scattering magnitude and directionality is attained with increasing number of nanocubes forming a linear chain. Optimal directionality, i.e., the narrowest main-scattering lobe, is found at the wavelength of interfering quadrupolar resonances; whereas the largest main-lobe magnitude is observed at the wavelength satisfying the first Kerkers condition. These unique optical properties of dielectric nanocubes thus can revolutionize their applications at visible and near-infrared regions in the fields of nanoantennas, nanolasers, photovoltaics, and even in biomedicine.

Two-Dimensional Bipyramid Plasmonic Nanoparticle Liquid Crystalline Superstructure with Four Distinct Orientational Packing Orders

Anisotropic plasmonic nanoparticles have been successfully used as constituent elements for growing ordered nanoparticle arrays. However, orientational control over their spatial ordering remains challenging. Here, we report on a self-assembled two-dimensional (2D) nanoparticle liquid crystalline superstructure (NLCS) from bipyramid gold nanoparticles (BNPs), which showed four distinct orientational packing orders, corresponding to horizontal alignment (H-NLCS), circular arrangement (C-NLCS), slanted alignment (S-NLCS), and vertical alignment (V-NLCS) of constituent particle building elements. These packing orders are characteristic of the unique shape of BNPs because all four packing modes were observed for particles with various sizes. Nevertheless, only H-NLCS and V-NLCS packing orders were observed for the free-standing ordered array nanosheets formed from a drying-mediated self-assembly at the air/water interface of a sessile droplet. This is due to strong surface tension and the absence of particle-substrate interaction. In addition, we found the collective plasmonic coupling properties mainly depend on the packing type, and characteristic coupling peak locations depend on particle sizes. Interestingly, surface-enhanced Raman scattering (SERS) enhancements were heavily dependent on the orientational packing ordering. In particular, V-NLCS showed the highest Raman enhancement factor, which was about 77-fold greater than the H-NLCS and about 19-fold greater than C-NLCS. The results presented here reveal the nature and significance of orientational ordering in controlling plasmonic coupling and SERS enhancements of ordered plasmonic nanoparticle arrays.

Effect of number density on optimal design of gold nanoshells for plasmonic photothermal therapy.

Despite much research efforts being devoted to the design optimization of metallic nanoshells, no account is taken of the fact that the number of the nanoshells that can be delivered to a given cancerous site vary with their size. In this paper, we study the effect of the nanoshell number density on the absorption and scattering properties of a gold-nanoshell ensemble exposed to a broadband near-infrared radiation, and optimize the nanoshells’ dimensions for efficient cancer treatment by analyzing a wide range of human tissues. We first consider the general situation in which the number of the delivered nanoshells decreases with their mean radius R as ∝ R−β, and demonstrate that the optimal design of nanoshells required to treat cancer most efficiently depends critically on β. In the case of β = 2, the maximal energy absorbed (scattered) by the ensemble is achieved for the same dimensions that maximize the absorption (scattering) efficiency of a single nanoshell. We thoroughly study this special case by the example of gold nanoshells with silica core. To ensure that minimal thermal injury is caused to the healthy tissue surrounding a cancerous site, we estimate the optimal dimensions that minimize scattering by the nanoshells for a desired value of the absorption efficiency. The comparison of gold nanoshells with different cores shows that hollow nanoshells exhibiting relatively low absorption efficiency are less harmful to the healthy tissue and, hence, are preferred over the strongly absorbing nanoshells. For each of the cases analyzed, we provide approximate analytical expressions for the optimal nanoshell dimensions, which may be used as design guidelines by experimentalists, in order to optimize the synthesis of gold nanoshells for treating different types of human cancer at their various growth stages.

Optimized gold nanoshell ensembles for biomedical applications

We theoretically study the properties of the optimal size distribution in the ensemble of hollow gold nanoshells (HGNs) that exhibits the best performance at in vivo biomedical applications. For the first time, to the best of our knowledge, we analyze the dependence of the optimal geometric means of the nanoshells’ thicknesses and core radii on the excitation wavelength and the type of human tissue, while assuming lognormal fit to the size distribution in a real HGN ensemble. Regardless of the tissue type, short-wavelength, near-infrared lasers are found to be the most effective in both absorption- and scattering-based applications. We derive approximate analytical expressions enabling one to readily estimate the parameters of optimal distribution for which an HGN ensemble exhibits the maximum efficiency of absorption or scattering inside a human tissue irradiated by a near-infrared laser.

Tunable Broadband Optical Responses of Substrate-Supported Metal/Dielectric/Metal Nanospheres

Using the image charge theory and finite element methods, we present the first comprehensive study on the optical properties of substrate-supported, three-layer, metal/dielectric/metal nanospheres. By adopting dipolar and quadrupolar approximations of the quasistatic image charge theory, we derive analytical expressions for the polarization-dependent polarizabilities of a three-layer nanosphere near a substrate and use them to find the nanosphere’s plasmon resonance wavelengths as functions of the geometric and material parameters of the nanosphere–substrate system. By calculating the resonance wavelength of substrate-supported gold/silica/gold nanosphere over a sufficiently large domain of the nanosphere’s dimensions, we show that this wavelength can be tuned from visible to infrared regions by altering only the size of the nanosphere’s core. We also show that the resonance position as well as the enhancement and confinement of the near-field can be dynamically tuned over broad ranges by changing the polarization of the excitation light. Of significance for the applicability of our results in practice is that we employ size-dependent permittivity of gold, which allows experimentalists to readily produce these substrate-supported nanospheres with desired optical responses. Upon comparing our analytical results with the results of numerical simulations, we reveal the range of the nanospheres’ outer radii within which the dipolar and quadrupolar approximations adequately describe the nanosphere–substrate interaction. Since majority of the optical functions are realized with light polarized parallel to the substrate, our results allow one to readily engineer the broadband optical responses of substrate-supported metal/dielectric/metal nanospheres for applications in resonance-enhanced sensing, in light harvesting, and in biomedicine.

Unveiling ultrasharp scattering–switching signatures of layered gold–dielectric–gold nanospheres

We study the light scattering profile of a subwavelength layered gold–dielectric–gold nanosphere, which unveils exciting ultrasharp scattering–switching signatures based on high spectral proximity of the scattering resonance and cloaking states. Analytical expressions are derived for polarizability, resonance/cloaking conditions, and for scattering cross section of this layered metal–dielectric–metal (MDM) nanosphere, under the quasi-static limit. Our analysis allows one to thoroughly investigate its spectral response, over the entire parametric space of its dimensions and the incident light wavelength. Especially, the scattering spectra reveal multiple Fano-type, ultrasharp spectral profiles with high tunability, in terms of abrupt scattering–switching wavelengths and cloaking bandwidth, when absorption losses in the metallic layers are neglected in the analysis. Upon inclusion of bulk metallic losses along with enhanced electron surface scattering effects, these sharp spectral signatures are found to get severely faded in a realistic layered MDM nanosphere. The results obtained analytically, in each case, are found to be in excellent agreement with the numerical ones calculated based on Mie theory. We demonstrate that the ultrasharp scattering signatures of a pragmatic MDM nanosphere can be revived by introducing semiconductor gain inclusions in the middle dielectric layer, mitigating losses in the metallic layers.

Matryoshka-caged gold nanorods: Synthesis, plasmonic properties, and catalytic activity

Matryoshka-caged gold nanorods (mCGNRs) were successfully synthesized by alternating between a seed-mediated silver-coating method and galvanic replacement reactions (GRRs). As the number of matryoshka layers of the mCGNRs increased, the plasmon resonance peak broadened and was red-shifted, and the catalytic activity towards the reduction of 4-nitrophenol (4-NTP) increased. When mCGNRs with 6 layers were used as nanocatalysts in the reduction of 4-nitrophenol, the reaction rate coefficient was 5.2- and 3.7-times higher than that of the gold-nanorod- and caged-gold-nanorod-catalyzed reductions of 4-nitrophenol, respectively. In addition, the surface-plasmon-resonance-based absorption of light enhanced the catalytic performance of the mCGNRs. With the support of a polyurethane foam, the mCGNRs synthesized in this study can be applied as recyclable heterogeneous catalysts for the reduction of 4-nitrophenol.

Theory of tailorable optical response of two-dimensional arrays of plasmonic nanoparticles at dielectric interfaces

Two-dimensional arrays of plasmonic nanoparticles at interfaces are promising candidates for novel optical metamaterials. Such systems materialise from ‘top–down’ patterning or ‘bottom–up’ self-assembly of nanoparticles at liquid/liquid or liquid/solid interfaces. Here, we present a comprehensive analysis of an extended effective quasi-static four-layer-stack model for the description of plasmon-resonance-enhanced optical responses of such systems. We investigate in detail the effects of the size of nanoparticles, average interparticle separation, dielectric constants of the media constituting the interface, and the nanoparticle position relative to the interface. Interesting interplays of these different factors are explored first for normally incident light. For off-normal incidence, the strong effects of the polarisation of light are found at large incident angles, which allows to dynamically tune the reflectance spectra. All the predictions of the theory are tested against full-wave simulations, proving this simplistic model to be adequate within the quasi-static limit. The model takes seconds to calculate the system’s optical response and makes it easy to unravel the effect of each system parameter. This helps rapid rationalization of experimental data and understanding of the optical signals from these novel ‘metamaterials’, optimised for light reflection or harvesting.

Gold nanoparticles with gain-assisted coating for ultra-sensitive biomedical sensing

We propose and theoretically demonstrate a scheme where ultra-sensitive biomedical sensing can be realized using a gold nanosphere with gain-assisted coating. Surface plasmon resonance (SPR) enhanced optical response of this coated nanoparticle is investigated using both quasi-static approximation limit analysis and exact Mie theory calculations. It is shown that a strongly SPR-amplified scattering efficiency accompanied by an extremely high quality factor of the plasmonic resonance can be achieved by introducing a relatively low level of gain into the coating layer. The application of such a gain-assisted coated gold nanoparticle in biomedical sensing is further investigated, which proves its ability to detect even marginal change in the concentration of its surrounding medium.