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From general relativity, to axionic-dark-matter-induced inflationary cosmology, and holographic graphenePierpoint, Michael P. January 2015 (has links)
This thesis explores the expansive world of General Relativity, and its role to play in modern cosmology and quantum field theory. We begin with a pedagogical approach to relativity, in particular, highlighting upon the ambiguity that arises with the conventions used in different textbooks. A brief introduction to tensor calculus has also been provided in the appendix. The preliminary chapters are also complimented with examples of numerical relativity via simulation. We then move on to discuss examples of non-linear systems, and their exact solutions. Such systems will be analogous to those we shall encounter later, upon considering scalar field theories as a means of modelling dark energy. We shall introduce the axion as our highly motivated dark matter candidate, since this will ultimately determine the behaviour of the scalar field. Coupled to a scaling factor across the spatial domain, it is found that this scalar field will ultimately determine the evolution of our universe. The key result of this thesis has been the possibility to screen both the cosmological constant, and flatness of the universe, to within observable parameters. These results will be explicitly derived from first principles. Also included is a tentative approach to holographic theory, in which strongly correlated systems may be modelled within the asymptotic domain of Anti-de Sitter (AdS) space. Ultimately, our aspirations are to bridge the gap with condensed matter theory, in particular with the publications included within the latter appendices. These publications discuss graphene as a revolutionary new material, for inclusion in both transistor-based and optoelectronic devices.
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The modification of graphene oxide and studies of the detection of norovirus DNA and RNALe, Duy Duc January 1900 (has links)
Master of Science / Department of Chemistry / Duy H. Hua / Graphene oxide (GO) has attracted many researchers in the past years because of its unique electrical and chemical properties which showed the potential applications in many fields such as electronic materials and biology. Increasing research efforts in the biomedical field are bringing to light new discoveries in areas such as drug delivery, treatment of cancers, and biosensors, and are therefore attractive.
The purpose of this work is to prepare GO and modify the surface of GO in order to achieve a new functionalized GO for biosensor applications in the future.
GO was synthesized from the flake graphite by using a modified Hummer’s method to achieve higher quality and yield. The flake graphite was first exfoliated by using a microwave reactor. The exfoliated flake graphite then was oxidized by K[subscript]2S[subscript]2O[subscript]8, P[subscript]2O[subscript]5, and KMnO[subscript]4 under acidic conditions, followed by H[subscript]2O[subscript]2 to form GO. The following steps were to attach carboxylic acid and benzoic acid groups onto the surface of GO. Atomic force microscopy (AFM), Fourier transform infrared spectroscopy (FTIR), and Raman spectroscopy were used to identity the modified GO and determine the sizes of the materials after a sequence of reactions. The modified GO will be used in the study of electronic sensing of biomolecules in Hua’s laboratory.
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Designing nanoscale constructs from atomic thin sheets of graphene, boron nitride and gold nanoparticles for advanced material applications.Jasuja, Kabeer January 1900 (has links)
Doctor of Philosophy / Department of Chemical Engineering / Vikas Berry / Nanoscale materials invite immense interest from diverse scientific disciplines as these provide access to precisely understand the physical world at their most fundamental atomic level. In concert with this aim of enhancing our understanding of the fundamental behavior at nanoscale, this dissertation presents research on three nanomaterials: Gold nanoparticles (GNPs), Graphene and ultra-thin Boron Nitride sheets (UTBNSs). The three-fold goals which drive this research are: incorporating mobility in nanoparticle based single-electron junction constructs, developing effective strategies to functionalize graphene with nano-forms of metal, and exfoliating ultrathin sheets of Boron Nitride.
Gold nanoparticle based electronic constructs can achieve a new degree of operational freedom if nanoscale mobility is incorporated in their design. We achieved such a nano-electromechanical construct by incorporating elastic polymer molecules between GNPs to form 2-dimensional (2-D) molecular junctions which show a nanoscale reversible motion on applying macro scale forces. This GNP-polymer assembly works like a molecular spring opening avenues to maneuver nano components and store energy at nano-scale.
Graphene is the first isolated nanomaterial that displays single-atom thickness. It exhibits quantum confinement that enables it to possess a unique combination of fascinating electronic, optical, and mechanical properties. Modifying the surface of graphene is extremely significant to enable its incorporation into applications of interest. We demonstrated the ability of chemically modified graphene sheets to act as GNP stabilizing templates in solution, and utilized this to process GNP composites of graphene. We discovered that GNPs synthesized by chemical or microwave reduction stabilize on graphene-oxide sheets to form snow-flake morphologies and bare-surfaces respectively. These hybrid nano constructs were extensively studied to understand the effect and nature of GNPs’ interaction with graphene, and applied to address the challenge of dispersing bare-surfaced GNPs for efficient liquid-phase catalysis. We also revisited the functionalization of graphene and present a non-invasive surface introduction of interfaceable moieties.
Isostructural to graphene, ultrathin BN sheet is another atomic-thick nanomaterial possessing a highly diverse set of properties inconceivable from graphene. Exfoliating UTBNSs has been challenging due to their exceptional intersheet-bonding and chemical-inertness. To develop applications of BN monolayers and evolve research, a facile lab-scale approach was desired that can produce processable dispersions of BN monolayers. We demonstrated a novel chlorosulfonic acid based treatment that resulted in protonation assisted layer-by-layer exfoliation of BN monolayers with highest reported yields till date. Further, the BN monolayers exhibited extensively protonated N centers, which are utilized for chemically interfacing GNPs, demonstrating their ability to act as excellent nano-templates.
The scientific details obtained from the research shown here will significantly support current research activities and greatly impact their future applications. Our research findings have been published in ACS Nano, Small, Journal of Physical Chemistry Letters, MRS Proceedings and have gathered >45 citations.
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Effects of graphene oxide nanoparticles on the immune system biomarkers produced by RAW 264.7Algadi, Hend Emhemed January 2019 (has links)
Magister Scientiae (Medical Bioscience) - MSc(MBS) / Graphene oxide (GO) is a single carbon layer, oxygen bearing graphene derivative, containing hydroxyl and carboxyl groups. Graphene oxide nanoparticles (GONPs) are promising nanomaterials for a variety of applications such as electrochemical analysis, adsorption of biomolecules, biosensors and drug and vaccine delivery systems. While these newly engineered nanoparticles hold great potential for developments in industry and medicine, the widespread use of these material will inevitably result in GO residues in the environment where they could possibly pose a risk to human and wildlife health. Interaction of the nanoparticles and biota can affect numerous biological processes. In humans they can affect any of the physiological systems such as the immune, endocrine, reproductive and cardiovascular systems. Although studies have indicated that GO exposure cause increased reactive oxygen species in cells, they mechanisms whereby GO act on the cell are still poorly understood. A few studies have investigated the effects of GONP and other graphene nanoparticle derivatives on the immune system. The aim of this study was to investigate the in vitro effects of GONPs on the immune system by the exposure of the murine macrophage cell line, RAW 264.7, to different concentrations of GONPs.
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Studies of two-dimensional materials beyond graphene: from first-principles to machine learning approachesHanakata, Paul Zakharia Fajar 12 July 2019 (has links)
Monolayers and heterostructures of two-dimensional (2D) electronic materials with spin-orbit interactions offer the promise of observing many novel physical effects. While theoretical predictions of 2D layered materials based on density functional theory (DFT) are many, the DFT approach is limited to small simulation sizes (several nanometers), and thus inhomogeneous strain and boundary effects that are often observed experimentally cannot be simulated within a reasonable time. The aim of this thesis is (i) to study effects of strain on 2D materials beyond graphene using first-principles and tight-binding methods and (ii) to investigate the effects of cuts--"kirigami"-- on 2D materials using molecular dynamics and machine learning approach.
The first half of this thesis focuses on the effects of strain on manipulating spin and valley degrees of freedom for two classes of 2D materials--monochalcogenide and lead chalcogenide monolayers--using DFT. A tight-binding (TB) approach is developed to describe the electronic changes in lead chalcogenide monolayers due to strains that often persist in real devices. The strain-dependent TB model allows one to establish a relationship between the Rashba field and the out-of-plane strain or electric polarization from a microscopic view, a connection that is not well understood in the ferroelectric Rashba materials. This framework connecting strain fields and electronic changes is important to overcome the size and computational limitations associated with DFT.
The second part of the thesis focuses on defect engineering and design of 2D materials via the "kirigami" technique of introducing different patterns of cuts. A machine learning (ML) approach is presented to provide physical insights and an effective model to describe the physical system. We demonstrate that a machine learning model based on a convolutional neural network is able to find the optimal design from a training data set that is much smaller than the design space.
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Nanoestruturas de óxido de grafeno magnético : modificação e funcionalização de superfície para terapia fotodinâmica e fototérmica /Paiva, Juliana Moreno de. January 2017 (has links)
Orientador: Rodrigo Fernando Costa Marques / Banca: Maria Aparecida Zaghethe Bertochi / Banca: Juliana Marchi / Resumo: As terapias fotodinâmica e fototérmica vêm sendo desenvolvidas de forma a oferecer melhores e mais baratas alternativas no tratamento de câncer. Os principais desafios na utilização destas técnicas estão na obtenção de novos materiais fototérmicos e fotosensibilizadores que absorvam no mesmo comprimento de onda. Neste contexto, este trabalho desenvolveu um material com este potencial. Para isso foi escolhido como base o óxido de grafeno devido suas propriedades hidrofílica e atóxica, boa estabilidade térmica, capacidade de absorção de luz e possibilidade de funcionalização. Nanopartículas de óxido de ferro magnéticas, floresceína o-metacrilato e o Verteporfin foram ligados em sua superfície trazendo novas características como a possibilidade do uso como agente de contraste no diagnóstico por ressonância magnética nuclear e terapia fotodinâmica. Para isso, estratégia de síntese foi feita em quatro etapas: síntese do óxido de grafeno, óxido de grafeno magnético, óxido de grafeno magnético fluorescente e óxido de grafeno magnético fluorescente com fotossenssibilizador. Na primeira etapa empregou-se o método de Hummers modificado para obtenção do óxido de grafeno pela oxidação e esfoliação do grafite. Em seguida, nanopartículas de óxido de ferro magnético foram imobilizadas em sua superfície pelo método de coprecipitação simples. A propriedade de fluorescência foi então inserida pela ancoragem da fluoresceína o-metacrilato juntamente com o ácido acrílico (AA), persulfato de amôni... (Resumo completo, clicar acesso eletrônico abaixo) / Photodynamic and photothermal therapies have been developed in order to offer better and cheaper alternatives in cancer treatment . The main challenges in the use of these techniques are in obtaining new photothermal and photosensitizers materials that absorb at the same wavelength. In this context, this work has developed a material with this potential. For this, graphene oxide was chosen as the base due to its hydrophilic and nontoxic properties, good thermal stability, light absorbing capacity and possibility of functionalization. Magnetic iron oxide nanoparticles, fluorescein o - methacrylate and Verteporfin were linked on their surface bringing new features such as the possibility of use as a contrast agent in the diagnosis by nuclear magnetic resonance and photodynamic. For this, the synthesis strategy was done in four steps: synthesis of gra phene oxide, magnetic graphene oxide, fluorescent magnetic graphene oxide and fluorescent magnetic graphene oxide with photosensitizer. In the first step, the modified Hummers method was used to obtain graphene oxide by t he oxidation and exfoliation of gra phite. Next, nanoparticles of magnetic iron oxide were immobilized on their surface by the simple co - precipitation method. The fluorescence property was then inserted by fluorescein o - methacrylate anchoring along with acrylic acid (AA), ammonium persulfate and sodium bisulfite. Finally, the graphene oxide was functionalized with the Verteporfin photosensitizer by a transesterification reaction. In order to verify the physical - chemical and structural character of the intermediates and final products of each step, characterization techniques were used, such as high - resolution scanning electron microscopy ( SEM ), X - ray diffractometry (XRD), RAMAN spectroscopy, Ultraviolet/ visible spectroscopy (UV - Vis), Fourier transform infrared spectroscopy (FTIR), fluorescence spectroscopy, zeta potential and dynamic light scattering (DLS). From the... / Mestre
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Aspects topologiques des dérivés du graphène / Topological Aspects of Graphene DerivativesDe gail, Raphaël 20 March 2014 (has links)
Ces dernières années, la physique de la matière condensée a connu une profonde révolution de concepts par la découverte de nombreuses phases de la matière qui ne sont pas classifiables à la Landau, c’est à dire par leur groupe de symétrie. Si les premiers travaux remontent à ceux des effets Hall quantiques (entier et fractionnaire), ce n’est que récemment, avec l’avènement du graphène et des isolants topologiques que les physiciens ont réalisé que ces phases de la matière ne nécessitent, dans l’absolu, ni champ magnétique, ni basse température, par opposition aux effets Hall quantiques précédemment cités. Ces nouveaux états de la matière sont caractérisés non pas par la géométrie du problème mais plutôt par la topologie. Ici donc, la forme précise du spectre électronique n’est pas importante, seules certaines caractéristiques, comme la présence ou l’absence d’un gap, le sont. De manière similaire à la classification de Landau des groupes de symétries, il est possible de classifier ces nouveaux systèmes par l’intermédiaire de groupes topologiques. La branche mathématique invoquée est celle de la topologie algébrique. A travers les invariants qu’elle génère, il est possible de classer les états topologiquement non-triviaux. De plus, les transitions entre des états à topologies distinctes sont aussi accessibles par cette théorie. Les travaux réalisés dans le cadre de cette thèse s’intéressent aux effets topologiques dans la structure de bandes de matériaux bi-dimensionnels. Après une présentation du formalisme mathématique général, un premier chapitre s’intéressera à la topologie locale, c’est à dire pour une portion restreinte de la première zone de Brillouin, des points de croisements de bandes, dits points de Dirac. Un effort sera porté vers la classification de ces systèmes et des transitions associées. Le chapitre suivant mettra en lumière un moyen efficace de mesurer les effets de la topologie des électrons en deux dimensions. Il s’agit de l’étude des niveaux de Landau qui résultent de l’application d’un champ magnétique 5transverse au plan des électrons. Les points de Dirac se transmutent alors en niveaux à énergie nulle topologiquement stables, c’est à dire peu ou pas influencés par les diverses perturbations. L’étude des différents modèles justifiera la discrimination entre la physique à champ magnétique faible et celle à champ magnétique fort, faible ou fort étant très dépendant du système étudié. Enfin, dans un dernier chapitre plus prospectif on s’intéressera à la topologie globale, c’est à dire pour l’ensemble de la première zone de Brillouin. Ce type d’étude est surtout caractérisé par l’existence d’états de bords robustes. On en fera l’expérience d’une double manière. D’abord par l’étude un modèle à un électron, puis par celle d’un système en forte interaction de N électrons. A travers les différents exemples étudiés, on s’attachera à démontrer la puissance de l’outil topologique pour les problèmes de la matière condensée, phénomène qui devrait s’accentuer les prochaines années. / During the last few decades, condensed matter physics has witnessed a deep refoundation of its paradigms, through the discovery of many systems that the usual symmety classification à la Landau cannot handle properly. Although the first major breaktroughs were realized at the time of discovery of integer and fractional quantum Hall effects, only recently physicists have agreed that these peculiar phases of matter require neither a magnetic field nor low temperature. Those new states of matter cannot be caracterized by the geometric aspects of the model but rather by topological ones. The precise shape of the electronic spectrum is no longer relevant, but only particular features are, such as the presence or the absence of a gap. Similarly to the Landau classification scheme, one can achieve a construction through extensive use of topological groups. This is the realm of algebraic topology. Related generated topological invariants can hold a classification of non-trivial topological states, as well as of the accompanying transitions. This thesis focusses on peculiar topological features of two-dimesnsional electronic band structures. After a technical introduction to the underlying formalism, the first chapter is devoted to local topology, that is for a restricted piece of the first Brillouin zone, of band crossing points, also known as Dirac points. Special care is taken to classify these points and related transitions. The next chapter sheds some light on a particularly efficent way of measuring topology for two-dimensional electrons. This is achieved through measurements of Landau levels that are generated by a magnetic field applied perpendicular to a plane. Dirac points then generate zero Landau levels that are topologically stable, i.e. almost not influenced by perturbations at all. Distinctions between low and high magnetic fields will prove to be relevant, although very system-dependant. Through the several models studied, we particularly stress out the importance of the topological tool for condensed matter physics, past present... and future.
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Estudo e desenvolvimento de sensores e dispositivos utilizando nanoestruturas alotrópicas de carbono / Study and development of sensors and devices based on nano-structured carbon allotropesSilva, Guilherme de Oliveira 10 July 2018 (has links)
Um desafio central na área das ciências da saúde e biomédica tem sido o desenvolvimento de testes clínicos embasados em novas tecnologias que resultem em medidas precisas, com resultados consistentes mais rápidos que os convencionais, e ao menor custo possível. Os esforços atuais têm se concentrado em integrar a análise de materiais biológicos a componentes de circuitos integrados compatíveis com a indústria de semicondutores existente. Nesse contexto, esse trabalho apresenta duas contribuições a partir do uso de materiais nanoestruturados alótropos do carbono. Primeiramente, demonstramos como o desempenho de um sensor de pH embasado na tecnologia EGFET (Extended Gate Field Effect Transistor) pode ser controlado com a incorporação de grafenos, com diferentes graus de funcionalização, a eletrodos de FTO (Fluorine doped Tin Oxide). Os eletrodos de FTO foram modificados através da deposição dos materiais nanoestruturados de carbono via eletroforese. O desempenho dessas amostras como sensor de íons H+ mostrou dependência quanto ao tempo de deposição e composição tampão utilizado, tendo seu desempenho aumentado em até 24%, atingindo uma sensibilidade máxima de 67 mVopH-1 para tampão fosfato. A segunda contribuição desse trabalho trata-se da combinação das informações obtidas com um arranjo de dispositivos de NTFETs (Nanotubes Field Effect Transitors) decorados com nanopartículas metálicas e análise de discriminantes lineares, empregados na classificação de diferentes populações celulares. O método proposto foi capaz de identificar e classificar corretamente entre as linhagens de células cancerígenas B16 (melanoma), 3LL (carcinoma) e 3L4 (linfoma), além de distingui-las corretamente de suas contrapartes saudáveis. Adicionalmente, utilizamos esse conjunto de dados para classificar uma população celular desconhecida, demonstrando uma possível utilidade clínica da metodologia desenvolvida. / A central challenge in the biomedical field has been the development of new approaches for clinical tests based on microelectronic technologies, aiming trustful and precise results, faster and cheaper than the standard techniques. Current efforts have focused on integrating the analysis of biological samples and integrated circuit components compatible with the standard semiconductor industry. In this context, the present work gives two contributions on the usage of carbon nanostructure allotropes. First, we show how the performance of pH sensors based on EGFET (Extended Gate Field Effect Transistor) can be tuned with the integration of graphene nanosheets, with different degrees of functionalization, into FTO (Fluorine doped Tin Oxide) electrodes. The FTO electrodes were modified through EPD (electrophoretic deposition) of the carbon nanomaterials. The device performance as pH sensor showed dependence on the time of deposition and buffer composition, increasing up to 24% compared to the bare FTO electrode and reaching a maximum sensitivity of 67 mVopH-1 for phosphate buffer. The second contribution of this work regard the combination of the data gathered using an array of NTFETs (Nanotube Field Effect Transistors) decorated with metal nanoparticles and LDA (Linear Discriminant Analysis) to distinguish among different cell populations. The proposed method correctly classifies among the cancer cell lines B16 (melanoma), 3LL (carcinoma), and 3L4 (lymphoma), as well as cancer cells from their healthy counterparts. Additionally, we demonstrated a possible application of the method correctly classifying blind samples.
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Caracterização de grafeno quimicamente esfoliado para aplicações em nanomedicina / Characterization of chemically exfoliated graphene for nanomedicine applicationsSantos, Fabrício Aparecido dos 24 October 2017 (has links)
Esta tese descreve a esfoliação e modificação do grafeno oxidado (GO) na obtenção de grafeno em sua forma reduzida (RGO) para aplicações biomédicas, que envolve sensoriamento e biossensoriamento, além de aplicação em fototerapia. Nas aplicações em sensores, inicialmente o RGO juntamente com o surfactante aniônico Dihexadecilfosfato (DHP), foi utilizado na fabricação de filmes por drop casting em eletrodo de carbono vítreo (CGE), na detecção do hormônio Estradiol. O eletrodo modificado (RGO-DHP/CGE) foi caracterizado por voltametria cíclica e impedância de espectroscopia eletroquímica. Os resultados mostraram uma corrente de pico de oxidação irreversível em 0,6 V. Sob as condições experimentais ideais, usando a voltametria linear, o limite de detecção para este hormônio foi de 7,7 × 10-8 mol L-1. Foram fabricados também dispositivos de efeito de campo (FET) de RGO via porta líquida em eletrodos interdigitados, para a detecção de Cistatina-C, um marcador de doença renal crônica. Os filmes foram fabricados utilizando a técnica de automontagem de interação eletrostática, nos quais, como polieletrólito de carga positiva foi utilizado o RGO modificado via ligação covalente de APTES, e como polieletrólito de carga negativa, o RGO dopado com nitrogênio, através da redução via micro-ondas. Estes dispositivos apresentaram uma sensibilidade de (1,94 ± 0,29) ΔIDS(%)ngmL-1. O LD foi de 0,39 ngmL-1 e a região linear entre 5 ngmL-1 100 ngmL-1, quando utilizados em urina sintética. Avaliamos também o uso de RGO em sistemas de fototerapia, utilizando GO reduzido com NH4OH na presença de L-Glutamina (RGO-Glu), onde observamos um aumento de temperatura localizado quando o material é irradiado por um laser (808 nm). Este sistema apresentou uma boa estabilidade e baixa agregação em dispersão aquosa e em meio de cultura, devido à formação de uma corona proteica. O RGO-Glu mostrou-se mais eficiente para o aquecimento que o RGO sem a modificação, na absorção do laser em 808 nm, com valores de eficiência de conversão de energia de 63% e 50% respectivamente. Estudos utilizando célula HeLa mostram que a internalização do RGO-Glu foi mais eficiente do que o RGO sem a modificação. Estes estudos mostram a versatilidade do grafeno quimicamente esfoliado em aplicações biomédicas quando convenientemente modificado, que pode ser utilizado em diagnóstico e em terapia. / This thesis describes the exfoliation and modification of graphene oxide (GO) to obtain reduced graphene oxide (RGO), for biomedical applications, namely: (bio)sensing for diagnostics and as active material in phototherapy. For (bio)sensing applications, RGO was used in combination with the anionic surfactant Dihexadecylphosphate (DHP) in the fabrication of drop-cast thin films onto carbon glass electrode (CGE), to be used in the detection of the hormone Estradiol. The modified electrode (RGO-DHP/CGE) was characterized by cyclic voltammetry and electrochemical spectroscopy impedance (EIS). The results showed an irreversible oxidation peak current at 0.6 V. Under ideal experimental conditions, and using linear voltammetry, the detection limit obtained for this sensor was 7.7 × 10-8 mol L-1. In the second part of the study, RGO was used in the fabrication of field effect transistors (FETs) via liquid gate, and the devices were applied in the detection of Cystatin-C, a biomarker for chronic renal disease. The films were made using the electrostatic layer-by-layer technique, in which APTES-modified RGO was used as positive polyelectrolyte, whereas nitrogen-doped RGO was used as the negative species. These devices exhibited a sensitivity of (1,94 ± 0,29) ΔIDS(%)ngmL-1, whereas LD was 0,39 ng.mL-1 and the linear region of detection was between 5 ng.mL-1 100 ngmL-1 when used in synthetic urine. The studies on the use of RGO in phototherapy were carried out using NH4OH -reduced GO in the presence of L-Glutamine (RGO-Glu) for subsequent cell internalization and irradiation under an 808 nm lase line to promote hiperthermia. This system showed good stability and low aggregation in aqueous dispersions and culture medium, due to the formation of a protein corona. RGO-Glu was more efficient than the RGO without the modification in the absorption of the laser at 808 nm, resulting in an efficiency of heat generation (energy conversion efficiency) of 63% and 50% respectively. Cytotoxicity studies using HeLa cell lines revealed that the internalization of RGO-Glu was more efficient than RGO without modification. These studies show the versatility of chemically exfoliated graphene oxides for biomedical applications, including diagnosis and therapy.
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Theory of Phonon Thermal Transport in Single-walled Carbon Nanotubes and GrapheneLindsay, Lucas R. January 2010 (has links)
Thesis advisor: David A. Broido / A theory is presented for describing the lattice thermal conductivities of graphene and single-walled carbon nanotubes. A phonon Boltzmann transport equation approach is employed to describe anharmonic phonon-phonon, crystal boundary, and isotopic impurity scattering. Full quantum mechanical phonon scattering is employed and an exact solution for the linearized Boltzmann transport equation is determined for each system without use of common relaxation time and long-wavelength approximations. The failures of these approximations in describing the thermal transport properties of nanotubes is discussed. An efficient symmetry based dynamical scheme is developed for carbon nanotubes and selection rules for phonon-phonon scattering in both graphene and nanotubes are introduced. The selection rule for scattering in single-walled carbon nanotubes allows for calculations of the thermal conductivities of large-diameter and chiral nanotubes that could not be previously studied due to computational limitations. Also due to this selection rule, no acoustic-only umklapp scattering can occur, thus, acoustic-optic scattering must be included in order to have thermal resistance from three-phonon processes. The graphene selection rule severely restricts phonon-phonon scattering of out-of-plane modes. This restriction leads to large contributions to the total thermal conductivity of graphene from the acoustic, out-of-plane modes which have been previously neglected. Empirical potentials used to model interactions in carbon-based materials are optimized to better describe the lattice dynamics of graphene-derived systems. These potentials are then used to generate the interatomic force constants needed to make calculations of the thermal conductivities of graphene and carbon nanotubes. Calculations of the thermal conductivities of single-walled carbon nanotubes and graphene for different temperatures and lengths are presented. The thermal conductivities of SWCNTs saturate in the diffusive regime when the effects of higher-order scattering processes are estimated and correctly reproduce the ballistic limit for short-length nanotubes at low temperatures. The effects of isotopic impurity scattering on the thermal conductivities of graphene and SWCNTs are explored. Isotopic impurities have little effect in the low (high) temperature regime where boundary (umklapp) scattering dominates the behavior of the thermal conductivities. In the intermediate temperature regime, modest reductions in the thermal conductivities, 15-20%, occur due to impurities. The thermal conductivities of a wide-range of SWCNTs are explored. The thermal conductivities of successively larger-diameter, one-dimensional nanotubes approach the thermal conductivity of two-dimensional graphene. / Thesis (PhD) — Boston College, 2010. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.
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