Engineering of electromagnetic interactions in three-dimensional plasmonic metamaterials

Thesis (Ph.D.)--Boston UniversityField of nanoplasmonics study the interaction of light with nanoscale metallic structures and it possesses the great potential of being the key element in future, highly integrated, on-chip nanophotonic aevices. Several major breakthroughs have been demonstrated in the past decade regarding the utilization of plasmonics for purposes ranging from optical nanoantennas to enhanced biochemical sensing platforms. So far, studies are generally focused on two-dimensional (2D) arrangement of plasmonic nanostructures. However, engineering of materials in three dimensions (3D) by integrating different kinds of plasmonic resonances in multi-layers, offers additional degrees of freedom in our design space, resulting in remarkable effects This thesis research investigates the outcomes of the tailoring of electromagnetic interactions between multiple plasmonic structures in three-dimensions. We are mainly focused on a coherence phenomenon termed as Farro resonance. Farro resonances are generally studied in atomic physics, which occur due to an interference between multiple excitation pathways where a discrete resonant state is coupled to a broad continuum. Fano resonances are inherently linked to an atomic physics concept termed as Electromagnetically Induced Transparency (EIT). Recently, a plasmonic analogue of the EIT effect was proposed and drew great attention. Plasmon Induced Transparency (PIT) enables one to mimic the extremely dispersive spectral characteristics of EIT, on-chip and without any stringent requirements. In the first two parts of this work, we show that by a precise engineering of the near-field interactions of plasmonic elements, PIT effect can be carried simultaneously to multiple spectral domains. This effect has many potential applications ranging from enhanced non-linearities to novel optical communication systems. In the third part, we investigate a multi-spectral Fano resonant plasmonic structure's non-linear response by embedding a nanoscale Kerr medium to the design. We show that a unique set of effects can be achieved through the interplay of Fano resonances and embedded optical non-linearity. In the last part, we develop a unifying theory to describe Fano resonances in both purely plasmonic structures and also in other systems which are comprised of plasmonic structures coupled to molecular resonances. The developed theory provides an invaluable intuition to Fano resonances and their utilization in applications such as biosensing and spectroscopy

A coupling model for quasi-normal modes of photonic resonators

We develop a model for the coupling of quasi-normal modes in open photonic systems consisting of two resonators. By expressing the modes of the coupled system as a linear combination of the modes of the individual particles, we obtain a generalized eigenvalue problem involving small size dense matrices. We apply this technique to dielectric rod dimmer of rectangular cross section for Transverse Electric (TE) polarization in a two-dimensional (2D) setup. The results of our model show excellent agreement with full-wave finite element simulations. We provide a convergence analysis, and a simplified model with a few modes to study the influence of the relative position of the two resonators. This model provides interesting physical insights on the coupling scheme at stake in such systems and pave the way for systematic and efficient design and optimization of resonances in more complicated systems, for applications including sensing, antennae and spectral filtering

Cascaded plasmon resonances for enhanced nonlinear optical response

The continued development of integrated photonic devices requires low-power, small volume all-optical modulators. The weak nonlinear optical response of conventional optical materials requires the use of high intensities and large interaction volumes in order to achieve significant light modulation, hindering the miniaturization of all-optical switches and the development of lightweight transmission optics with nonlinear optical response. These challenges may be addressed using plasmonic nanostructures due to their unique ability to confine and enhance electric fields in sub-wavelength volumes. The ultrafast nonlinear response of free electrons in such plasmonic structures and the fast thermal nonlinear optical response of metal nanoparticles, as well as the plasmon enhanced nonlinear Kerr-type response of the host material surrounding the nanostructures could allow ultrafast all-optical modulation with low modulation energy. In this thesis, we investigate the linear and nonlinear optical response of engineered effective media containing coupled metallic nanoparticles. The fundamental interactions in systems containing coupled nanoparticles with size, shape, and composition dissimilarity, are evaluated analytically and numerically, and it is demonstrated that under certain conditions the achieved field enhancement factors can exceed the single-particle result by orders of magnitude in a process called cascaded plasmon resonance. It is demonstrated that these conditions can be met in systems containing coupled nanospheres, and in systems containing non-spherical metal nanoparticles that are compatible with common top-down nanofabrication methods such as electron beam lithography and nano-imprint lithography. We show that metamaterials based on such cascaded plasmon resonance structures can produce enhanced nonlinear optical refraction and absorption compared to that of conventional plasmonic nanostructures. Finally, it is demonstrated that the thermal nonlinear optical response of metal nanoparticles can be enhanced in carefully engineered heterogeneous nanoparticle clusters, potentially enabling strong and fast thermal nonlinear optical response in system that can be produced in bulk through chemical synthesis

Plasmonic Nanoplatforms for Biochemical Sensing and Medical Applications

Plasmonics, the science of the excitation of surface plasmon polaritons (SPP) at the metal-dielectric interface under intense beam radiation, has been studied for its immense potential for developing numerous nanophotonic devices, optical circuits and lab-on-a-chip devices. The key feature, which makes the plasmonic structures promising is the ability to support strong resonances with different behaviors and tunable localized hotspots, excitable in a wide spectral range. Therefore, the fundamental understanding of light-matter interactions at subwavelength nanostructures and use of this understanding to tailor plasmonic nanostructures with the ability to sustain high-quality tunable resonant modes are essential toward the realization of highly functional devices with a wide range of applications from sensing to switching. We investigated the excitation of various plasmonic resonance modes (i.e. Fano resonances, and toroidal moments) using both optical and terahertz (THz) plasmonic metamolecules. By designing and fabricating various nanostructures, we successfully predicted, demonstrated and analyzed the excitation of plasmonic resonances, numerically and experimentally. A simple comparison between the sensitivity and lineshape quality of various optically driven resonances reveals that nonradiative toroidal moments are exotic plasmonic modes with strong sensitivity to environmental perturbations. Employing toroidal plasmonic metasurfaces, we demonstrated ultrafast plasmonic switches and highly sensitive sensors. Focusing on the biomedical applications of toroidal moments, we developed plasmonic metamaterials for fast and cost-effective infection diagnosis using the THz range of the spectrum. We used the exotic behavior of toroidal moments for the identification of Zika-virus (ZIKV) envelope proteins as the infectious nano-agents through two protocols: 1) direct biding of targeted biomarkers to the plasmonic metasurfaces, and 2) attaching gold nanoparticles to the plasmonic metasurfaces and binding the proteins to the particles to enhance the sensitivity. This led to developing ultrasensitive THz plasmonic metasensors for detection of nanoscale and low-molecular-weight biomarkers at the picomolar range of concentration. In summary, by using high-quality and pronounced toroidal moments as sensitive resonances, we have successfully designed, fabricated and characterized novel plasmonic toroidal metamaterials for the detection of infectious biomarkers using different methods. The proposed approach allowed us to compare and analyze the binding properties, sensitivity, repeatability, and limit of detection of the metasensing device

Dielectric nanostructures for control of electromagnetic waves

High refractive index dielectric nanoantennas have emerged as a promising unit for improving optical nanodevices by compensating the drawbacks of plasmonic nanoantennas, which have played a key role in nanophotonics to date. The features of high refractive index dielectric nanoantennas, such as low energy losses, excitation of strong magnetic resonances and enhancement of electric field inside and outside the particle, are expected to provide novel methods to manipulate electromagnetic waves in the nanometer scale. In this thesis, we theoretically explore and experimentally demonstrate a variety of nanostructures based on high refractive index dielectric nanoantennas to aim at the efficient and tuneable control of electromagnetic waves in linear and nonlinear manners. Firstly, asymmetric Si dimers are investigated to achieve unidirectional forward scattering with high efficiency. An electric or magnetic dipole mode is excited in each particle constituting the asymmetric dimer at the same wavelength. The interference between these two dipolar modes can direct the scattered field selectively into the forward direction with high scattering efficiency. Secondly, we investigate metasurfaces built of array of Si nanodimers to obtain switching from high transmission to reflection depending on the incident polarization. The different linear polarization direction of the incident light can alter the hybridization modes of the constituent Si dimers and, hence, the effective permittivity and permeability of the metasurface. The resulted overlap and separation of the electric and magnetic dipolar resonances facilitates the control over the switching between high transmission and reflection. Thirdly, asymmetric Si dimers are explored to obtain tuneable control of directional scattering either in the left or right direction from the incident axis. Our theoretical analysis reveals that the electric or magnetic dipoles excited perpendicular to the dimer axis are mainly responsible for the tuneable scattering. Experimental demonstration of the scattering tuneability is carried out along the substrate by using back focal plane techniques combined with a prism coupling setup. Fourthly, we show that the third harmonic generation from a high refractive index dielectric nanoantenna can be significantly improved by adding a metallic component to build a metal-dielectric hybrid nanostructure. In this way, the plasmonic resonance of a Au nanoring can boost the anapole mode excited in a Si nanodisk, strongly enhancing the electric field inside the Si nanodisk. As a result, high third harmonic intensity and conversion efficiency can be achieved even in nanometer scale. Our findings on how we can attain the efficient and tuneable control of electromagnetic waves using high refractive index dielectric nanostructures will contribute to opening the new paths towards the realization of novel optical nanodevices.Open Acces

Recent Advances in Linear and Nonlinear Optics

Sight is the dominant sense of mankind to apprehend the world at the earth scale and beyond the frontiers of the infinite, from the nanometer to the incommensurable. Primarily based on sunlight and natural and artificial light sources, optics has been the major companion of spectroscopy since scientific observation began. The invention of the laser in the early sixties has boosted optical spectroscopy through the intrinsic or specific symmetry electronic properties of materials at the multiscale (birefringence, nonlinear and photonic crystals), revealed by the ability to monitor light polarization inside or on the surface of designed objects. This Special Issue of Symmetry features articles and reviews that are of tremendous interest to scientists who study linear and nonlinear optics, all oriented around the common axis of symmetry. Contributions transverse the entire breadth of this field, including those concerning polarization and anisotropy within colloids of chromophores and metal/semiconducting nanoparticles probed by UV-visible and fluorescence spectroscopies; microscopic structures of liquid–liquid, liquid–gas, and liquid–solid interfaces; surface- and symmetry-specific optical techniques and simulations, including second-harmonic and sum-frequency generations, and surface-enhanced and coherent anti-Stokes Raman spectroscopies; orientation and chirality of bio-molecular interfaces; symmetry breaking in photochemistry; symmetric multipolar molecules; reversible electronic energy transfer within supramolecular systems; plasmonics; and light polarization effects in materials

Fano resonance assisting plasmonic circular dichroism from nanorice heterodimers for extrinsic chirality

In this work, the circular dichroisms (CD) of nanorice heterodimers consisting of two parallel arranged nanorices with the same size but different materials are investigated theoretically. Symmetry-breaking is introduced by using different materials and oblique incidence to achieve strong CD at the vicinity of Fano resonance peaks. We demonstrate that all Au-Ag heterodimers exhibit multipolar Fano resonances and strong CD effect. A simple quantitative analysis shows that the structure with larger Fano asymmetry factor has stronger CD. The intensity and peak positions of the CD effect can be flexibly tuned in a large range by changing particle size, shape, the inter-particle distance and surroundings. Furthermore, CD spectra exhibit high sensitivity to ambient medium in visible and near infrared regions. Our results here are beneficial for the design and application of high sensitive CD sensors and other related fields