The objective of this study is to examine core-shell type plasmonic metamaterials aimed at the development of materials with unique electromagnetic properties. The building blocks of metamaterials under study consist of gold as a metal component, and silica and precipitated calcium carbonate (PCC) as the dielectric media. The results of this study demonstrate important applications of the core-shells including scattering suppression, airborne obscurants made of fractal gold shells, photomodification of the fractal structure providing windows of transparency, and plasmonics core-shell with a gain shell as an active device. Plasmonic resonances of the metallic shells depend on their nanostructure and geometry of the core, which can be optimized for the broadband extinction. Significant extinction from the visible to mid-infrared makes fractal shells very attractive as bandpass filters and aerosolized obscurants. In contrast to the planar fractal films, where the absorption and reflection equally contribute to the extinction, the shells' extinction is caused mainly by the absorption. This work shows that the Mie scattering resonance of a silica core with 780 nm diameter at 560 nm is suppressed by 75% and only partially substituted by the absorption in the shell so that the total transmission is noticeably increased. Effective medium theory supports …

In this work, we study the use of a spatial light modulator (SLM) for local manipulation of phase in interfering laser beams to fabricate photonic crystal templates with embedded, engineered defects. A SLM displaying geometric phase patterns was used as a digitally programmable phase mask to fabricate 4-fold and 6-fold symmetric photonic crystal templates. Through pixel-by-pixel phase engineering, digital control of the phases of one or more of the interfering beams was demonstrated, thus allowing change in the interference pattern. The phases of the generated beams were programmed at specific locations, resulting in defect structures in the fabricated photonic lattices such as missing lattice line defects, and single-motif lattice defects in dual-motif lattice background. The diffraction efficiency from the phase pattern was used to locally modify the filling fraction in holographically fabricated structures, resulting in defects with a different fill fraction than the bulk lattice. Through two steps of phase engineering, a spatially variant lattice defect with a 90° bend in a periodic bulk lattice was fabricated. Finally, by reducing the relative phase shift of the defect line and utilizing the different diffraction efficiency between the defect line and the background phase pattern, desired and functional defect lattices can be …

We investigate the conditions under which electron irradiation of single-walled carbon nanotube (SWCNT) bundles with 2 keV electrons produces an increase in the Raman D peak. We find that an increase in the D peak does not occur when SWCNTs are preheated in situ at 600 C for 1 h in ultrahigh vacuum (UHV) before irradiation is performed. Exposing SWCNTs to air or other gases after preheating in UHV and before irradiation results in an increase in the D peak. Small diameter SWCNTs that are not preheated or preheated and exposed to air show a significant increase in the D and G bands after irradiation. X-ray photoelectron spectroscopy shows no chemical shifts in the C1s peak of SWCNTs that have been irradiated versus SWCNTs that have not been irradiated, suggesting that the increase in the D peak is not due to chemisorption of adsorbates on the nanotubes.

Among the well-known methods to form or modify the composition and physical properties of thin films, ion implantation has shown to be a very powerful technique. In particular, ion beam syntheses of binary iron silicide have been studied by several groups. Further, the interests in transition metal silicide systems are triggered by their potential use in advanced silicon based opto-electronic devices. In addition, ternary silicides have been by far less studied than their binary counterparts despite the fact that they have interesting magnetic and electronic properties. In this study, we investigate ion beam synthesis of Fe-Si binary structures and Fe-Co-Si ternary structures. This work involves fundamental investigation into development of a scalable synthesis process involving binary and ternary transitional metal silicide thin films and Nano-structures using low energy ion beams. Binary structures were synthesized by implanting Fe- at 50 keV energy. Since ion implantation is a dynamic process, Dynamic simulation techniques were used in these studies to determine saturation fluences for ion implantation. Also, static and dynamic simulation results were compared with experimental results. The outcome of simulations and experimental results indicate, dynamic simulation codes are more suitable than static version of the TRIM to simulate high fluence, low energy …

Fractional calculus enables the possibility of using real number powers or complex number powers of the differentiation operator. The fundamental connection between fractional calculus and subordination processes is explored and affords a physical interpretation for a fractional trajectory, that being an average over an ensemble of stochastic trajectories. With an ensemble average perspective, the explanation of the behavior of fractional chaotic systems changes dramatically. Before now what has been interpreted as intrinsic friction is actually a form of non-Markovian dissipation that automatically arises from adopting the fractional calculus, is shown to be a manifestation of decorrelations between trajectories. Nonlinear Langevin equation describes the mean field of a finite size complex network at criticality. Critical phenomena and temporal complexity are two very important issues of modern nonlinear dynamics and the link between them found by the author can significantly improve the understanding behavior of dynamical systems at criticality. The subject of temporal complexity addresses the challenging and especially helpful in addressing fundamental physical science issues beyond the limits of reductionism.

We study the behavior of electric fields in and around dielectric and metal nanoparticles, and prepare the ground for their applications to a variety of systems viz. photovoltaics, imaging and detection techniques, and molecular spectroscopy. We exploit the property of nanoparticles being able to focus the radiation field into small regions and study some of the interesting nonlinear, and quantum coherence and interference phenomena near them. The traditional approach to study the nonlinear light-matter interactions involves the use of the slowly varying amplitude approximation (SVAA) as it simplifies the theoretical analysis. However, SVVA cannot be used for systems which are of the order of the wavelength of the light. We use the exact solutions of the Maxwell's equations to obtain the fields created due to metal and dielectric nanoparticles, and study nonlinear and quantum optical phenomena near these nanoparticles. We begin with the theoretical description of the electromagnetic fields created due to the nonlinear wavemixing process, namely, second-order nonlinearity in an nonlinear sphere. The phase-matching condition has been revisited in such particles and we found that it is not satisfied in the sphere. We have suggested a way to obtain optimal conditions for any type and size of material medium. …

This dissertation work is a study of the growth kinematics, synthesis strategies and intrinsic properties of InSb nanowires (NWs). The highlights of this work include a study of the effect of the growth parameters on the composition and crystallinity of NWs. A change in the temperature ramp-up rate as the substrate was heated to reach the NW growth temperature resulted in NWs that were either crystalline or amorphous. The as-grown NWs were found to have very different optical and electrical properties. The growth mechanism for crystalline NWs is the standard vapor-liquid-solid growth mechanism. This work proposes two possible growth mechanisms for amorphous NWs. The amorphous InSb NWs were found to be very sensitive to laser radiation and to heat treatment. Raman spectroscopy measurements on these NWs showed that intense laser light induced localized crystallization, most likely due to radiation induced annealing of defects in the region hit by the laser beam. Electron transport measurements revealed non-linear current-voltage characteristics that could not be explained by a Schottky diode behavior. Analysis of the experimental data showed that electrical conduction in this material is governed by space charge limited current (SCLC) in the high bias-field region and by Ohm's law in the low …

Understanding the fundamental physics in light absorption and perfect light absorption is vital for device applications in detector, sensor, solar energy harvesting and imaging. In this research study, a large area fabrication of Al-doped ZnO/Al2O3/graphene/Al2O3/gold/silicon device was enabled by a spin-processable hydrophilic mono-layer graphene oxide. In contrast to the optical properties of noble metals, which cannot be tuned or changed, the permittivity of transparent metal oxides, such as Al-doped ZnO and indium tin oxide, are tunable. Their optical properties can be adjusted via doping or tuned electrically through carrier accumulation and depletion, providing great advantages for designing tunable photonic devices or realizing perfect absorption. A significant shift of Raman frequency up to 360 cm-1 was observed from graphene in the fabricated device reported in this work. The absorption from the device was tunable with a negative voltage applied on the Al-doped ZnO side. The generated absorption change was sustainable when the voltage was off and erasable when a positive voltage was applied. The reflection change was explained by the Fermi level change in graphene. The sustainability of tuned optical property in graphene can lead to a design of device with less power consumption.

This thesis is an attempt at studying quantum coherence effects coupled via plasmons. After introducing the quantum coherence in atomic systems in Chapter 1, we utilize it in Chapter 2 to demonstrate a new technique of detection of motion of single atoms or irons inside an optical cavity. By taking into account the interaction of coherences with surface plasmonic waves excited in metal nanoparticles, we provide a theoretical model along with experimental data in Chapter 3 to describe the modification of Raman spectra near metal nanoparticles. We show in chapter 4 that starting from two emitters, coupled via a plasmonic field, the symmetry breaking occurs, making detectable the simultaneous existence of the fast super-radiance and the slow sub-radiance emission of dye fluorescence near a plasmonic surface. In Chapter 5, we study the photon statistics of a group of emitters coupled via plasmons and by the use of quantum regression theorem, we provide a theoretical model to fully investigate the dependence of photon bunching and anti-bunching effects to the interaction between atoms, fields and surrounding mediums.

In this dissertation, I am presenting my research on the fabrication and simulation of the optical properties of 3D photonic crystals and 2D graded photonic super-crystals. The 3D photonic crystals were fabricated using holographic lithography with a single, custom-built reflective optical element (ROE) and single exposure from a visible light laser. Fully 3D photonic crystals with 4-fold, 5- fold, and 6-fold symmetries were fabricated using the flexible, 3D printed ROE. In addition, novel 2D graded photonic super-crystals were fabricated using a spatial light modulator (SLM) in a 4f setup for pixel-by-pixel phase engineering. The SLM was used to control the phase and intensity of sets of beams to fabricate the 2D photonic crystals in a single exposure. The 2D photonic crystals integrate super-cell periodicities with 4-fold, 5-fold, and 6-fold symmetries and a graded fill fraction. The simulations of the 2D graded photonic super-crystals show extraordinary properties such as full photonic band gaps and cavity modes with Q-factors of ~106. This research could help in the development of organic light emitting diodes, high-efficiency solar cells, and other devices.

The performance of electrical and optical devices based on two-dimensional semiconductors (2D) such as molybdenum disulfide is critically influenced due to very poor light absorption in the atomically thin layers. In this study, the phonon mediated optical absorption and emission properties in single atomic layers of MoS2 have been investigated. The electronic transitions in MoS2 due to near-field optical interaction and the influence of interface phonons due to the dielectric substrate GaN on the relaxation of optically generated carriers will be described. The near-field interaction can be induced in the presence of metal plasmons deposited on the surface of MoS2 monolayers. A hybrid metal-semiconductor system was realized by the deposition of silver (Ag) NPs on MoS2 layer and the localized plasmon modes were selectively chosen to interact with quasiparticles such as excitons and phonons. These quasiparticles are confined within the single atomic layer of MoS2 and are stable at room temperatures due to high binding energy. The lattice vibrational modes in MoS2 can be optically excited with the pulses from a femtosecond laser. These phonon modes can be optically dressed due to near-field interaction in the hybrid Ag-MoS2 system under an optical excitation resonant to localized plasmon modes. The coherent …

The effects of surface plasmon for InGaN/GaN multi-quantum wells and ZnO nanoparticles optical linear and nonlinear emission efficiency had been experimentally studied. Due to the critical design for InGaN MQWs with inverted hexagonal pits based on GaN, both contribution of surface plasmon effect and image charge effect at resonant and off resonant frequencies were experimentally and theoretically investigated. With off- resonant condition, the InGaN MQWs emission significantly enhanced by metal nanoparticles. This enhancement was caused by the image charge effect, due to the accumulation of carriers to NPs region. When InGaN emission resonated with metal particles SP modes, surface Plasmon effect dominated the emission process. We also studied the surface plasmon effect for ZnO nanoparticles nonlinear optical processes, SHG and TPE. Defect level emission had more contribution at high incident intensity. Emissions are different for pumping deep into the bulk and near surface. A new assumption to increase the TPE efficiency was studied. We thought by using Au nanorods localized surface plasmon mode to couple the ZnO virtual state, the virtual state’s life time would be longer and experimentally lead the emission enhancement. We studied the TPE phenomena at high and near band gap energy. Both emission intensity and decay …

Many social, biological and technological systems can be viewed as complex networks with a large number of interacting components. However despite recent advancements in network theory, a satisfactory description of dynamic processes arising in such cooperative systems is a subject of ongoing research. In this dissertation the emergence of dynamical complexity in networks of interacting stochastic oscillators is investigated. In particular I demonstrate that networks of two and three state stochastic oscillators present a second-order phase transition with respect to the strength of coupling between individual units. I show that at the critical point fluctuations of the global order parameter are characterized by an inverse-power law distribution and I assess their renewal properties. Additionally, I study the effect that different types of perturbation have on dynamical properties of the model. I discuss the relevance of those observations for the transmission of information between complex systems.

Broad band light emission ranging from the ultraviolet (UV) to the near infrared (NIR) has been observed from silicon nanoparticles fabricated using low energy (30-45 keV) metal and non-metal ion implantation with a fluence of 5*1015 ions/cm2 in crystalline Si(100). It is found from a systematic study of the annealing carried out at certain temperatures that the spectral characteristics remains unchanged except for the enhancement of light emission intensity due to annealing. The annealing results in nucleation of metal nanoclusters in the vicinity of Si nanoparticles which enhances the emission intensity. Structural and optical characterization demonstrate that the emission originates from both highly localized defect bound excitons at the Si/Sio2 interface, as well as surface and interface traps associated with the increased surface area of the Si nanocrystals. The emission in the UV is due to interband transitions from localized excitonic states at the interface of Si/SiO2 or from the surface of Si nanocrystals. The radiative efficiency of the UV emission from the Si nanoparticles can be modified by the localized surface plasmon (LSP) interaction induced by the nucleation of silver nanoparticles with controlled annealing of the samples. The UV emission from Si nanoclusters are coupled resonantly to the LSP …

Poly ethylene glycol (PEG) based microgels were synthesized and investigated. The PEG microgel has the same phase transition as the traditional poly N-isopropylacrylamide (PNIPAM). As a good substitute of PNIPAM, PEG microgel exhibits many advantages: it is easier to control the lower critical solution temperature (LCST) of the microgel by changing the component of copolymers; it has a more solid spherical core-shell structure to have a double thermo sensitivity; it is straightforward to add other sensitivities such as pH, magnetic field or organic functional groups; it readily forms a photonic crystal structure exhibiting Bragg diffraction; and, most importantly, the PEG microgel is biocompatible with human body and has been approved by FDA while PNIPAM has not. PEG microgels with core-shell structure are synthesized with a two-step free radical polymerization and characterized with DLS, SLS and UV–Vis. The dynamic mechanics of melting and recrystallizing of the PEG core-shell microgel are presented and discussed. Photonic crystals of PEG microgels were synthesized and characterized. The crystal can be isolated in a thin film or a bulk column. The phase transition of PEG microgel was simulated with the mean field theory. The enthalpy and entropy of phase transition can be estimated from the best …

The use of nuclear microprobe techniques including: Particle induced x-ray emission (PIXE) and Rutherford backscattering spectrometry (RBS) for elemental analysis and quantitative elemental imaging of biological samples is especially useful in biological and biomedical research because of its high sensitivity for physiologically important trace elements or toxic heavy metals. The nuclear microprobe of the Ion Beam Modification and Analysis Laboratory (IBMAL) has been used to study the enhancement in metal uptake of two different plants. The roots of corn (Zea mays) have been analyzed to study the enhancement of iron uptake by adding Fe (II) or Fe (III) of different concentrations to the germinating medium of the seeds. The Fe uptake enhancement effect produced by lacing the germinating medium with carbon nanotubes has also been investigated. The aim of this investigation is to ensure not only high crop yield but also Fe-rich food products especially from calcareous soil which covers 30% of world’s agricultural land. The result will help reduce iron deficiency anemia, which has been identified as the leading nutritional disorder especially in developing countries by the World Health Organization. For the second plant, Mexican marigold (Tagetes erecta), the effect of an arbuscular mycorrhizal fungi (Glomus intraradices) for the …

The electrical and optical properties of boron doped hydrogenated amorphous silicon thin films (a-Si) were investigated to determine the effect of boron and hydrogen incorporation on carrier transport. The a-Si thin films were grown by plasma enhanced chemical vapor deposition (PECVD) at various boron concentrations, hydrogen dilutions, and at differing growth temperatures. The temperature dependent conductivity generally follows the hopping conduction model. Above a critical temperature, the dominant conduction mechanism is Mott variable range hopping conductivity (M-VRH), where p = ¼, and the carrier hopping depends on energy. However, at lower temperatures, the coulomb interaction between charge carriers becomes important and Efros-Shklosvkii variable hopping (ES-VRH) conduction, where p=1/2, must be included to describe the total conductivity. To correlate changes in electrical conductivity to changes in the local crystalline order, the transverse optical (TO) and transverse acoustic (TA) modes of the Raman spectra were studied to relate changes in short- and mid-range order to the effects of growth temperature, boron, and hydrogen incorporation. With an increase of hydrogen and/or growth temperature, both short and mid-range order improve, whereas the addition of boron results in the degradation of short range order. It is seen that there is a direct correlation between the …

Synthesis and capture of antihydrogen in controlled laboratory conditions will enable precise studies of neutral antimatter. The work presented deals with some of the physics pertinent to manipulating charged antiparticles in order to create neutral antimatter, and may be applicable to other scenarios of plasma confinement and charged particle interaction. The topics covered include the electrostatic confinement of a reflecting ion beam and the transverse confinement of an ion beam in a purely electrostatic configuration; the charge sign effect on the Coulomb logarithm for a two component (e.g., antihydrogen) plasma in a Penning trap as well as the collisional scattering for binary Coulomb interactions that are cut off at a distance different than the Debye length; and the formation of magnetobound positronium and protonium.

Angular distributions and total yields of atoms sputtered from bismuth targets by normally incident 10 keV -50 keV Ne+ and Ar+ ions have been measured both experimentally and by computer simulation. Polycrystalline Bi targets were used for experimental measurements. The sputtered atoms were collected on high purity aluminum foils under ultra-high vacuum conditions, and were subsequently analyzed using Rutherford backscattering spectroscopy. The Monte-Carlo based SRIM code was employed to simulate angular distributions of sputtered Bi atoms and total sputtering yields of Bi to compare with experiment. The measured sputtering yields were found to increase with increasing projectile energy for normally incident 10 keV - 50 keV Ne+ and Ar+ ions. The shapes of the angular distributions of sputtered Bi atoms demonstrated good agreement between experiment and simulation in the present study. The measured and simulated angular distributions of sputtered Bi exhibited an over-cosine tendency. The measured value of the degree of this over-cosine nature was observed to increase with increasing incident Ne+ ion energy, but was not strongly dependent on incident Ar+ ion energy. The differential angular sputtering yield and partial sputtering yields due to Ar ion bombardment of an inhomogeneous liquid Bi:Ga alloy have been investigated, both experimentally and …

Semi-conductor industry relies heavily on silicon (Si). However, Si is not a direct-band gap semi-conductor. Consequently, Si does not possess great versatility for multi-functional applications in comparison with the direct band-gap III-V semi-conductors such as GaAs. To bridge this gap, what is ideally required is a semi-conductor material system that is based on silicon, but has significantly greater versatility. While sparsely studied, the semi-conducting silicides material systems offer great potential. Thus, I focused on the growth and structural characterization of ruthenium silicide and osmium silicide material systems. I also characterized iron silicon germanide films using extended x-ray absorption fine structure (EXAFS) to reveal phase, semi-conducting behavior, and to calculate nearest neighbor distances. The choice of these silicides material systems was due to their theoretically predicted and/or experimentally reported direct band gaps. However, the challenge was the existence of more than one stable phase/stoichiometric ratio of these materials. In order to possess the greatest control over the growth process, molecular beam epitaxy (MBE) has been employed. Structural and film quality comparisons of as-grown versus annealed films of ruthenium silicide are presented. Structural characterization and film quality of MBE grown ruthenium silicide and osmium silicide films via in situ and ex situ …

Positronium-hydrogen (Ps-H) scattering is of interest, as it is a fundamental four-body Coulomb problem. We have investigated low-energy Ps-H scattering below the Ps(n=2) excitation threshold using the Kohn variational method and variants of the method with a trial wavefunction that includes highly correlated Hylleraas-type short-range terms. We give an elegant formalism that combines all Kohn-type variational methods into a single form. Along with this, we have also developed a general formalism for Kohn-type matrix elements that allows us to evaluate arbitrary partial waves with a single codebase. Computational strategies we have developed and use in this work will also be discussed.With these methods, we have computed phase shifts for the first six partial waves for both the singlet and triplet states. The 1S and 1P phase shifts are highly accurate results and could potentially be viewed as benchmark results. Resonance positions and widths for the 1S-, 1P-, 1D-, and 1F-waves have been calculated.We present elastic integrated, elastic differential, and momentum transfer cross sections using all six partial waves and note interesting features of each. We use multiple effective range theories, including several that explicitly take into account the long-range van der Waals interaction, to investigate scattering lengths for the 1,3S …

Functional materials are essential to human welfare and to provide foundations for emerging industries. As an alternative route to experimental materials discovery, computational materials designs are playing an increasingly significant role in the whole discovery process. In this work, we use an in-house developed python utility: PAOFLOW, which generates finite basis Hamiltonians from the projection of first principles plane-wave pseudopotential wavefunctions on pseudo atomic orbitals(PAO) for post-process calculation on various properties such as the band structures, density of states, complex dielectric constants, diffusive and anomalous spin and charge transport coefficients. In particular, we calculated the dielectric function of Sr-, Pb-, and Bi-substituted BaSnO3 over wide concentration ranges. Together with some high-throughput experimental study, our result indicates the importance of considering the mixed-valence nature and clustering effects upon substitution of BaSnO3 with Pb and Bi. We also studied two prototype ferroelectric rashba semiconductors, GeTe and SnTe, and found the spin Hall conductivity(SHC) can be large either in ferroelectric or paraelectric structure phase. Upon doping, the polar displacements in GeTe can be sustained up to a critical hole concentration while the tiny distortions in SnTe vanish at a minimal level of doping. Moreover, we investigated the sensitivity of two dimensional group-IV monochalcogenides …

A nuclear microprobe, typically consisting of 2 - 4 quadrupole magnetic lenses and apertures serving as objective and a collimating divergence slits, focuses MeV ions to approximately 1 x 1 μm for modification and analysis of materials. Although far less utilized, electrostatic quadrupole fields similarly afford strong focusing of ions and have the added benefit of doing so independent of ion mass. Instead, electrostatic quadrupole focusing exhibits energy dependence on focusing ions. A heavy ion microprobe could extend the spatial resolution of conventional microprobe techniques to masses untenable by quadrupole magnetic fields. An electrostatic quadrupole doublet focusing system has been designed and constructed using several non-conventional methods and materials for a wide range of microprobe applications. The system was modeled using the software package "Propagate Rays and Aberrations by Matrices" which quantifies system specific parameters such as demagnification and intrinsic aberrations. Direct experimental verification was obtained for several of the parameters associated with the system. Details of the project and with specific applications of the system are presented.

Various anomalous effects that emerge when the interfaces between media are involved in sound-matter or light-matter interactions are studied. The three specific systems examined are a fluid channel between elastic metal plates, a linear chain of metallic perforated cylindrical shells in air, and a metal-dielectric slab with the interfaces treated as finite regions of smoothly changing material properties. The scattering of acoustic signals on the first two is predicted to be accompanied by the effects of redirection and splitting of sound. In the third system, which supports the propagation of surface plasmons, it is discovered that the transition region introduces a nonradiative decay mechanism which adds to the plasmon dissipation. The analytical results are supported with numerical simulations. The outlined phenomena provide the ideas and implications for applications involving manipulation of sound or excitation of surface plasmons.