Nano-reinforced polymeric systems have demonstrated a great deal of interest within academia and industry, due to the intrinsic properties of the graphene nanofillers, having excellent mechanical, thermal and electrical properties. The reinforcement of multiwall carbon nanotubes (MWCNTs) and graphene nanoplatelets (GNPs) were introduced into a low cost, non-carcinogenic, high temperature PMR type polyimide resin. The effects of the interfacial interaction and dispersion quality resulted in improvement in the glass transition temperature (Tg), elastic modulus and thermal stability by, 31°C, 63% and 16°C, respectively. In fine, this study presents a simple but effective high temperature polyimide (HTPI) nanocomposites manufacturing procedure and established that nanoparticle reinforcement can be used to improve both thermal and mechanical properties. / Includes bibliography. / Thesis (M.S.)--Florida Atlantic University, 2018. / FAU Electronic Theses and Dissertations Collection

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This thesis presents a detailed study of chip based silicon photonic waveguide technologies for chemical sensing applications. The project specifically focuses on the use of strip and slot waveguide based micro-ring resonators (MRRs) integrated with graphene and graphene oxide (GO) as potential functional sensor coatings. The primary objective is to understand the effect of graphene/GO on the optical properties of such a device, to assess performance in bio-/chemical sensing applications and to identify ways in which such a device may be optimised. A detailed analysis of how the MRR cavity optical extinction ratio (ER) varies with the interaction length of surface integrated graphene reveals, for the first time using this technique, the in-plane graphene linear absorption coefficient, αgTE = 0.11 ± 0.01dBμm⁻¹. A model of the MRR cavity optical losses for different graphene lengths and heights (above the waveguide surface) provides a predictive capability for the design rules of optimised performance in sensing and photo-detector based applications. The graphene integrated MRRs were also characterized by a Raman mapping technique from which careful analysis of the graphene G and 2D scattering peak frequencies and relative intensities revealed that the graphene is electrically intrinsic where it is suspended over the MRR yet moderately hole-doped where it sits on top of the waveguide structure. This 'pinning' of the graphene Fermi level at the graphene-silicon/SiO2 interface is the result of 'trapped' ad-charges, the concentration of which may be increased at dangling bond sites after relatively aggressive (O2 plasma) cleaning of the silicon/SiO2 surface prior to graphene transfer. Quantifying this substrate doping effect is critically important when attempting to determine graphene's optical properties and should be taken into account when designing graphene-silicon hetero-structures for opto-electronic devices. The large absorption coefficient determined for the graphene integrated MRR devices means that cavity losses are far too high for practical realisation of refractive index based sensing. However, an alternative approach using GO as the functional layer for improved MRR based refractive index sensors remains a possibility on account of the much lower transmission loss. GO also has distinct advantages over graphene; ease of integration, a high density of surface functional groups and micro-porosity. Transmission spectral analyses of both bare (uncoated) MRRs and those coated with different GO concentrations revealed the in-plane linear absorption coefficient for the GO film to be αGOTE = 0.027±0.02dBμm⁻¹, which is much lower than that for graphene. Construction of a gas cell and integrated 'bubbler' arrangement for delivering variable vapour concentrations to the graphene/GO integrated MRR devices under test is presented. Both bare and GO coated MRRs were exposed to vapours from a series of typical organic solvents; ethanol, pentene and acetone delivered by a carrier gas (N2). Dynamic optical tracking of the MRR cavity resonance wavelength during vapour exposure, at different flow rates (vapour concentrations) reveals the sensitivity of the device(s) to small changes in refractive index. The dynamic response of the GO coated MRRs to the vapours were up to three times faster than the uncoated MRR with similar improvements in sensitivity and limit of detection, largely attributable to the porous nature and molecular binding affinity of the GO. Critically, these experiments reveal that the detection sensitivity and response of the GO is solvent dependent, which may mean that it is capable of providing a degree of selectivity, which is normally difficult to achieve in refractive index based gas sensing.

This thesis presents novel results in the field of plasmonics and optoelectronics application. Plasmonics is the rapidly expanding branch of photonics. It opens up capabilities of electronic and photonic device implementation within the same integrated circuits as well as enhances the limit of detection for chemical and biological-based sensors. The first finding lies in solving the dilemma in search of ultimate plasmonics materials for plasmonics application. It is well known that Cu and Ag are metals that have incredible electric and optic properties. However, they are easily oxidized in contact with air. Both experimental and theoretical findings demonstrate that application of a mono or bilayer graphene protects Cu and Ag from oxidation and degradation of its plasmonic properties. The performance of each metal is evaluated based on the quality factor Q and the minima in amplitude of reflection intensity Rmin of the Surface plasmon-polariton (SPP) curve. The second novelty of this thesis comprises the fabrication of low loss, high efficient broadband, as well as narrowband, graphene-based electro-absorption modulators. The studied graphene-based modulators made use of Fabry-Perot resonator geometries. It has been shown that high-k dielectric hafnium dioxide (HfO2) provides solid state “supercapacitor” effects and allows to observe light modulation from the near-infrared to shorter wavelengths close to the visible spectrum with remarkably low gate voltages (~4 V). The electro-absorption modulators based on Fabry-Perot resonator geometry reached the modulation depth in transmission mode of 28% at a wavelength of 1.1 Âμm.

In this thesis, the synthesis and characterization of nitrogen-doped graphene (NG) and NG-Co3O4 composites are described. Moreover, the effect of airborne contamination and nitrogen doping on the capacitance of graphene was investigated. Firstly, nitrogen-doped thermally expanded graphene oxide (NtGO) was prepared by a facile thermal expansion and hydrothermal doping process. The thermal expansion process plays a vital role in improving the electrochemical performance of N-doped graphene by preventing its aggregation and improving its conductivity. The specific capacitance of NtGO is 270 F g-1 at a discharge current density of 1 A g-1 and the capacitance retention is 97 % after 2000 cycles at this current density. Secondly, a hierarchical electrode structure, consisting of cobalt oxide and nitrogen-doped graphene foam (NGF), has been fabricated with the aim of achieving enhanced charge storage performance. The Co3O4/NGF electrode shows an enhanced charge-storage performance, attributed to the 3D hierarchical structure and the synergistic effect of Co3O4 and NGF. The present study shows that specific capacitances as high as 451 F g-1 can be obtained, indicating that high-performance electrochemical capacitors can be made using electrode materials with advanced structures. Thirdly, a study of the differences between the capacitance of freshly exfoliated highly ordered pyrolytic graphite (HOPG, sample denoted FEG), HOPG aged in air (denoted AAG) and aged in an inert atmosphere (hereafter IAG) is presented in this work. Electrochemical impedance spectroscopy shows the FEG possesses a higher intrinsic capacitance (6.0 µF cm-2 at the potential of minimum capacitance) than AAG (4.3 µF cm-2) and IAG (4.7 µF cm-2). This change in capacitance is correlated with other physical changes of the sample, and attributed to contamination due to airborne hydrocarbons. Finally, the effect of N-doping of graphene prepared by chemical vapour deposition is investigated. The differential capacitance of PG and NG was measured by a microinjection-micromanipulator system. The quantum capacitance of PG and NG was calculated and discussed. The increase in differential capacitance with nitrogen-doping and the growth of the quantum capacitance of NG suggest that the increased capacitance of many electrodes of electrochemical capacitors is primarily due to the modification of the electronic structure of the graphene by the N dopant.

Ever since the discovery of carbon nano materials like carbon nanotube (CNT) and graphene, this class of materials has gained significant attention due to their exotic properties. The principle idea of my present research project is to understand the novel improvements induced in polymer matrices with inclusion of the nanofillers. This thesis is thematically divided into three parts. In the first part we introduce principle materials that we use for preparation of composites. Methods of nanofiller preparation and different nanocomposites as previously reported in literature are discussed to formulate the basis of our study. Different dispersion techniques are discussed which facilitate uniform nanofiller distribution. A variety of experimental methods are described which were employed to investigate the structure and properties of the composites. In the second part we discuss in details polyamide-12 (PA12) composites using CNT and graphene as fillers. A marked improvement is recorded in the toughness of the films with incorporation of CNT, dispersed in PA12 using a surfactant. Electrical percolation is also achieved in the otherwise insulating matrix. With PA-12 fibers we explored the effect of fiber processing and CNT incorporation in the mechanical properties. Extensive wide angle x-ray diffraction was carried out to interpret the structural modifications brought about by CNT in the matrix. The final part of the thesis deals with a thermosetting polymer, epoxy composites. CNT, Graphene and also a mixture of the two nanofillers were used as reinforcing agents. Appreciable improvement was recorded in the mechanical properties, electrical and thermal conductivity of the composites. Detailed optical and electron microscopy was carried out to get a vivid idea of the micro-structure and dispersion. The presented work demonstrates the significant ability of carbon nanofillers to reinforce polymer matrices enhancing their mechanical, electrical and thermal properties and opening a wide horizon for a variety of applications.

Increasing energy demand makes the development of higher energy storage batteries, imperative. However, one of the major advantages of fossil fuels as an energy source is they can provide variably large quantities of power when desired. This is where electrochemical capacitors can continue to carve out a niche market supplying moderate energy storage, but with high specific power output. However, current issues with carbon precursors necessitate further development. Further, production requires high temperature, energy intensive carbonization to create the active pore sites and develop the pores. Double-layer capacitive materials researched to replace active carbons generally require properties that include: very high surface area, high pore accessibility and wettability, strong electrical conductivity, structural stability, and optionally reversible functional groups that lend to energy storage through pseudocapacitive mechanisms. In recent years, nanostructured carbon materials which could in future be tailored through bottom up processing have the potential to exhibit favourable properties have also contributed to the growth in this field. This thesis presents research on graphene, an emerging 2-dimensional carbon material. So far, production of graphene in bulk exhibits issues including restacking, structural damage and poor exfoliation. However, the high chemical stability, moderate conductivity and high electroactive behaviour even with moderate exposed surface area makes them an excellent standalone material or a potential support material. Two projects presented focus on enhancing the capacitance through functionality and controlling graphene formation to enhance performance. The first study addresses graphene enhancement possible with heteroatom functionality, produced by a single step low temperature hydrothermal reduction process. The dopant methodology was successful in adding nitrogen functionality to the reduced graphene oxide basal and the effect of nitrogen type was considered. The second study addresses the need for greater control of the rGO structure on the macro-scale. By harnessing the change in interactions between the GO intermediate and final rGO sheets we were able to successfully control the assembly of graphene, creating micro and macro-pore order and high capacitive performance. Further, self assembly directly onto the current collector eliminates process steps involved in the production of EDLC electrodes.

In this study, we aimed to investigate the magnetic properties of the Co/graphene/Pt(111). Firstly, we used the annealing technique to prepare graphene. The car- bon atoms were segregated from the bulk of the Pt(111) to form graphene eager on the surface. After the preparation of graphene, we confirmed its quality by using STM and LEED. Secondly, we deposited 3 to 25 ML (monolayer) Co on graphene/Pt(111) by electron beam evaporator at low temperature ( 200 K). Then, we measured the ferromagnetic properties of different thickness of Co on graphene / Pt(111) by XMCD, and studied the growth behavior of few monolayer Co on graphene by STM. By serial analysis no ferromagnetic property of few monolayer Co was detected on graphene / Pt(111) by X-ray absorption spectra. The STM image show that the few monolayer Co on graphene mucleates as clusters.

Stable passive mode-locked fiber lasers(MLFLs) employing graphene saturable absorber (SA) are demonstrated. The graphene were dispersed in de-ionized water by two different dispersants including fluorinated mica clay (Mica) and poly(oxyethylene)-segmented imide (POEM). Using the SA made by graphene dispersed in Mica with thickness and concentration product (TCP) of 36 (£gm*wt%), the MLFLs exhibited pulsewidth, 3-dB spectral bandwidth, and modulation depth (MD) of 382 fs, 6.80 nm, and 2.57%, respectively. The graphene dispersed in POEM provides a TCP of 38 (£gm*wt%) to make the MLFLs deliver pulsewidth, 3-dB spectral bandwidth, and MD of 422 fs, 6.35 nm, and 1.70%, respectively. In comparison, the graphene SA dispersed by Mica performs a better MLFL pulse quality than that dispersed by POEM. Lastly, for investigating the dispersed uniformity between Mica and POEM, we randomly chose 9 pieces and measured the MLFL performance. The result showed that using the SA made by graphene dispersed in Mica with TCP of 36 (£gm*wt%), the MLFLs exhibited pulsewidth of 393¡Ó14 fs, By contrast, the graphene dispersed in POEM provided a TCP of 38 (£gm*wt%) to make the MLFLs delivered pulsewidth of 442¡Ó32 fs. This result reveals that graphene SA film dispersed by Mica exhibited better uniformity than POEM. The MLFL of 21-layes CVD process graphene SA showed a pulsewidth of 432.47 fs, a bandwidth of 6.16nm, and a time-bandwidth product (TBP) of 0.323. This result showed that the solution blending process graphene SA exhibited better MLFL performance than CVD.

Since its discovery in 2004, graphene has been widely touted as a potential replacement for silicon in the next generation of electronic circuits owing to its exceptionally high carrier mobilities and its ultra-thin body. Graphene field effect transistors (GFETs) show promising potential for use in analog and radio frequency (RF) applications, with theoretically predicted THz frequencies only being limited by fabrication challenges. High series resistance of the source/drain access regions in a GFET is one such major factor responsible for performance degradation. In this thesis, a simple and straightforward scheme of reducing this resistance by self-aligned spin-on-doping of graphene using surface transfer dopants is presented. Back-gated GFETs were fabricated on Si/SiO2 and doped using various surface transfer dopants. A novel method of spin-on-doping graphene using poly(ethyleneimine) (PEI) was developed. Top-gated GFETs with mobilities up to 6,900 cm2/Vs were fabricated and their access regions were spin-on-doped in a self-aligned manner offering a 3X reduction in the series resistance. GFET drive currents improved by up to 4X and transconductances up to 3X after self-aligned doping. GFETs were also fabricated on insulating quartz substrates with mobilities up to 5,600 cm2/Vs and showed performance enhancements up to 2X after self-aligned doping. / text