The recent discoveries of topological insulators (TI) has opened a new realm for study¬ing topological systems and exploring the exotic properties they offer. The in-built topological protection against direct backscattering and absence of localization makes two-dimensional (2D) surface states of bismuth chalcogenide-based strong TI a promising platform for studying interesting phenomena in condensed matter physics like dissipation-less transport, quantum anomalous hall effect, topological magnetoelectric effect, majo¬rana fermions etc. and also makes this system very suitable for applications in the fields of electronics and spintronics. However, realization of these novel states can be difficult because of scattering of surface states from different types of disorders (intrinsic or ex¬trinsic) or the presence of parallel channels in the bulk of the sample which can dominate over surface transport. The main goal of this thesis is to evaluate the performance of TI as an electronic element and look into elastic and inelastic scattering processes and kinetics of these scatterers. In most part of this work we concentrate on the magnitude and origin of low-frequency flicker noise or the 1/f-noise, a key performance marker in electronics, to characterize the electrical transport in TI. In this work we have studied 1/f-noise in both mechanically exfoliated TI-flakes and epitaxially grown TI films by varying chemical potential and temperature. Our study of exfoliated TI-flakes with a wide range of thickness (10 nm to 80 μm) suggests that whereas at thinner (<100 nm) samples and at low temperature (<70 K), the electrical transport happens entirely at the surface, resistance fluctuations in the surface states are mainly caused by potential fluctuations caused by generation-recombination processes in the bulk of TI. Study of 1/f-noise in MBE-grown magnetically doped TI reveals signature of hopping transport through localized bulk mid gap states. These states can either be Cr-impurity band or disorder-induced mobility edge states of bulk valence band. Our study of quantum transport in exfoliated TI-devices indicate presence of a de-coherence mechanism which saturates phase-coherence length and temperature below T< 3 K and results from a unique scattering mechanism caused by localized magnetic moments in these systems

Cette thèse s’inscrit dans le cadre du développement de nouveaux matériaux permettant de se substituer aux métaux pour les applications de transport de l’électricité. L’excellente conductivité électriques des nanotubes de carbone (NTC) ainsi que le fait qu’ils peuvent être assemblés sous forme de fil en font une alternative prometteuse. Cependant, la conductivité électrique des fils en NTC n’est pas encore suffisante pour directement concurrencer les métaux. Ce travail de thèse cherche à identifier et comprendre les points bloquants pour les dépasser et ainsi améliorer la conductivité des fils en NTC. Les nanotubes de carbones sont fabriqués par la technique de Chemical Vapour Deposition sous forme de tapis. Ces tapis dit "filable" permettent d'extraire une nappe de NTC que l’on densifie ensuite pour former un fil. Tous les travaux de la littérature sur ce type de fil rapportent des résistivités supérieures à 1 mΩ.cm. Afin de comprendre cette limite apparente, une étude approfondie du transport électronique de ces fils est présentée en étudiant le comportement de la résistance du matériau entre 3 K et 300 K. Cette analyse met en évidence que le transport dans les fils de NTC est dominé par les contacts entre NTC en dessous de 70 K et qu’il est dominé par le transport intrinsèque des NTC au-dessus de 70 K. L'amélioration de la conductivité des fils en NTC à température ambiante passe par l’amélioration de la conductivité intrinsèque des NTC. Pour ce faire, deux techniques sont présentées dans ce travail, l’amélioration de la qualité structurale des NTC obtenue par un recuit à plus de 2000 °C et le dopage. L'amélioration linéaire de la conductivité du fil de NTC avec la qualité structurale des NTC nous a permis d’atteindre un record de résistivité à 0.76 mΩ.cm. Le dopant présenté dans ce travail (PtCl4) est pour la première fois utilisé pour des fils en NTC. Ce dopant possède une excellente efficacité (résistivité diminuées par 3) et une très grande stabilité dans le temps. L’amélioration de la qualité structurale des NTC augmente fortement l’efficacité de dopage. La qualité structurale est indispensable pour atteindre d’excellentes conductivités électriques. Un schéma récapitule l’influence des différents paramètres expérimentaux sur le transport électronique des fils en NTC. Enfin, l’étude du transport électronique dans les matériaux en NTC a permis de développer un nouveau modèle de transport s’ajustant à la fois à nos travaux ainsi qu’à tous ceux de la littérature. Ce modèle consiste en deux résistances en série. La première résistance décrit le transport dans les matériaux en NTC en dessous de 70 K et est très bien décrite par la théorie d’un Liquide de Luttinger. La deuxième résistance dépend à la fois du transport intrinsèque des parois métalliques et semi-conductrices des NTC ainsi que de l’arrangement des NTC entre eux (faisceaux ou individualisés). Ce modèle permet de tirer les informations intrinsèques aux fils comme la façon dont les électrons sont injectés dans les NTC, l’influence des NTC semi-conducteurs par rapport aux métalliques et les libres parcours moyen des électrons dans la structure. L’ensemble de ces résultats indique que les paramètres indispensables pour obtenir des fils très conducteurs sont pour des NTC: d’une excellente qualité structurale, fabriqué sous forme individualisée et avec une forte proportion de parois métalliques. / The overall framework of this PhD. work is to develop new materials to replace metals in electrical wiring. Carbon nanotubes (CNT) are a good alternative as they show a high electrical conductivity as well as they can be assembled into yarns. However, CNT yarns have not yet reached the electrical conductivity of individual CNTs preventing them from competing with metals. The aim of this work is to identify the factors limiting the CNT yarn conductivity, increase the CNT yarn conductivity and model their electrical transport. In this work, carbon nanotubes are grown in array by Chemical Vapour Deposition. Our CNT arrays are spinnable meaning that, CNT webs can be drawn from it and then densified into yarns. All the published works on this type of CNT yarns reveal that their resistivities are limited above 1 mΩ.cm. In order to understand this apparent limitation, we present an extensive study of the CNT yarn electrical transport by measuring the yarn resistance behavior from 3 K to 300 K. We show that the CNT yarn electrical transport is dominated by the contact resistance between CNTs below 70 K and by the intrinsic CNT resistance above. In order to improve the CNT yarn electrical conductivity at room temperature, it is essential to improve the intrinsic CNT conductivity. Two ways are investigated, the first one is to increase the CNT structural quality by annealing above 2000 °C, and the second one is doping. Annealing treatment drastically improves the CNT structural quality, revealing that the CNT yarn resistivity linearly decreases with the CNT quality improvement. This treatment allows reaching a resistivity record of 0.76 mΩ.cm for undoped yarn made from CNT array. In addition, we present a new dopant for CNT yarn (PtCl4) that shows both high doping efficiency (CNT resistivity decreased by almost a factor of 3) and a very long term stability. By combining successively annealing and doping treatments, we found out that the doping efficiency is drastically increased by the CNT structural quality improvement. From all our experimental studies and the literature data analysis, we present a scheme showing the influence of many parameters on the CNT yarn electrical transport. After bringing to light that existing electrical transport models do not correctly explain the CNT yarn electrical transport, we developed a new model that perfectly fits both our data and those of the literature. Our model consists in two resistances in series. The first resistance represents the CNT material electrical transport below 70 K and is very well explained by the Luttinger Liquid theory. The second resistance depends on both the intrinsic CNT wall electrical transport (metallic or semi-conducting) and the CNT arrangement (bundled or individualized). Our model allows extracting CNT yarn physical parameters such as the way electrons tunnel from one CNT to another, the role of semi-conducting walls versus metallic ones and the electron mean free paths in the structure. All these results highlight that the main ways to make CNT yarns with high electrical conductivities involve individualized CNTs, with an excellent structural quality and also a high metallic CNT wall content.

In schwach gekoppelten Halbleiterübergittern können die Elektronen resonant von dem untersten Subband eines Quantentopfes in verschiedene höhere Subbänder des benachbarten Topfes durch die Potenzialbarriere tunneln. In stark dotierten Übergittern kann sich eine Ladungsakkumulationsschicht im Übergitter ausbilden, die es in zwei Felddomänen mit verschiedenen Feldstärken teilt. Aus der detaillierten Untersuchung des Stromverhaltens bei schnellen Spannungsänderungen konnten wichtige Erkenntnisse über die Dynamik der Akkumulationsschicht gewonnen werden, die zum besseren Verständnis von selbstgenerierten Stromoszillationen beitragen. Die beobachteten Stromoszillationen liegen in einem Frequenzbereich von einigen hundert kHz bis zu einigen GHz. Es werden zwei Oszillationsmoden ausführlich beschrieben und gezeigt, wie man sie unterscheiden kann. Die erste Mode tritt bei Proben mit einer gut leitenden Kontaktschicht und moderater Dotierung auf, bei denen die Feldverteilung im Übergitter instabil ist. Die zweite Mode kann dagegen auch bei stark dotierten Übergittern auftreten. Die Voraussetzung ist, dass die Emitterkontaktschicht einen genügend großen spezifischen Widerstand besitzt. Mit dem dargestellten Escape-Time-Modell kann man aus den Übergitterparametern die Oszillationsfrequenzen und die zu erwartenden Stromdichten in den verschiedenen Plateaus abschätzen. Weiterhin wird gezeigt, wie sich die äußere Beschaltung auf die Eigenschaften auswirkt. Durch den Einbau des Übergitters in einen Resonator können diskrete Frequenzen mit einem konstanten Frequenzabstand erzeugt werden. In der Arbeit wird auch der Einfluss von DX-Zentren in den Kontaktschichten beschrieben, welche die Eigenschaften der Proben bei tiefen Temperaturen stark beeinträchtigen können. Durch die Verbesserung der Probeneigenschaften oszilliert der Strom in den Übergittern auch bei Raumtemperatur. Die Frequenz ist mit Hilfe der angelegten Spannung innerhalb eines Plateaus kontinuierlich um bis zu einem Faktor vier durchstimmbar. Es wird die Verwendung von Oszillatoren, basierend auf schwach gekoppelten Halbleiterübergittern, als Bauelement für die Nachrichtenübermittlung vorgeschlagen. / In weakly coupled semiconductor superlattices, the electrons can resonantly tunnel from the first subband of a quantum well into a higher subband of the adjacent well. In highly doped superlattices, a charge accumulation layer can be formed, which divides the superlattice in two field domains of different field strengths. From detailed investigations of the current transients after fast voltage switches, one can obtain important insights into the dynamics of the accumulation layer, which is important for the understanding of self-sustained current oscillations. The frequencies of the resulting current oscillations of the investigated samples are in the range between several hundred kHz and a few GHz. Two possible oscillation modes and their identification from the oscillation characteristics are described. The first mode is observed in samples with contacts with a small resistance and moderately doped superlattices with an unstable field distribution. The second mode appears, if the resistance of the emitter contact layer is sufficiently large and a depletion layer can be injected. A semiclassical model is introduced for the estimation of the oscillation frequencies and the current density in the different plateaus from the superlattice parameters. Finally, the influence of the electrical circuit on the properties of the oscillations will be shown. If the superlattice is put into a resonator, discrete frequencies with constant distances are observed. In this thesis also the influences of DX-centers in the contact layers are described, which can significantly alter the properties of the samples at low temperatures. By applying a larger voltage or by illumination, the contact resistance can be recovered to a common value. Due to the improvement of the sample parameters, the samples also oscillate at room temperature and above. The frequency within a plateau is continuously tunable by a factor of two to four. An application as a tunable oscillator device for wireless and optical communication is proposed.

This thesis presents several experiments, generally aiming at visualising the ballistic and topological transport on the high-mobility graphene/boron nitride heterostructure using the scanning gate microscope. For the first experiment, we use the scanning gate microscopy to map out the trajectories of ballistic carriers in high-mobility graphene encapsulated by hexagonal boron nitride and in a weak perpendicular magnetic field. We employ a magnetic focusing transport configuration to image carriers that emerge ballistically from an injector, follow a cyclotron path due to the Lorentz force from an applied magnetic field, and land on an adjacent collector probe. The local potential generated by the scanning tip in the vicinity of the carriers deflects their trajectories, modifying the proportion of carriers focused into the collector. By measuring the voltage at the collector while scanning the tip, we are able to obtain images with arcs that are consistent with the expected cyclotron motion. We also demonstrate that the tip can be used to redirect misaligned carriers back to the collector. For the second experiment, we investigate the graphene van der Waals structures formed by aligning monolayer graphene with insulating layers of hexagonal boron nitride which exhibit a moiré superlattice that is expected to break sublattice symmetry. However, despite an energy gap of several tens of millielectronvolts opening in the Dirac spectrum, electrical resistivity remains lower than expected at low temperature and varies between devices. While subgap states are likely to play a role in this behaviour, their precise nature is still unclear in the community. We therefore perform a scanning gate microscopy study of graphene moiré superlattice devices with comparable activation energy but with different charge disorder levels. In the device with higher charge impurity ($\sim$ 10$^-$ cm$^{-2}$) and lower resistivity ($\sim$ 10 k$\Omega$) at the Dirac point we observe scanning gate response along the graphene edges. Combined with simulations, our measurements suggest that enhanced edge doping is responsible for this effect. In addition, a device with low charge impurity ($\sim$ 10$^{9}$ cm$^{-2}$) and higher resistivity ($\sim$ 100 k$\Omega$) shows subgap states in the bulk. Our measurements provide alternative model to the prevailing theory in the literature in which the topological bandstructures of the graphene moiré superlattices entail an edge currents shunting the insulating bulk. In the third experiment, we continue our study in the graphene moir$\acute e$ superlattices with the newly reported non-local Hall signals at the main Dirac point. It has been associated with the non-zero valley Berry curvature due to the gap opening and the nonlocal signal has been interpreted as the signature of the topological valley Hall effects. However, the nature of such signal is still disputed in the community, due to the vanishing density of states near the Dirac point and the possible topological edge transport in the system. Various artificial contribution without a topological origin of the measurement scheme has also been suggested. In connection to the second experiment, we use the scanning gate microscope to image the non-local Hall resistance as well as the local resistance in the current path. By analysing the features in the two sets of images, we find evidence for topological Hall current in the bulk despite a large artificial components which cannot be distinguished in global transport measurement. In the last experiment, we show the development of a radio-frequency scanning impedance microscopy compatible with the existing scanning gate microscopy and the dilution refrigerator. We detailed the design and the implementation of the radio-frequency reflectometry and the specialised tip holder for the integration of the tip and the transmission lines. We demonstrate the capability of imaging local impedance of the sample by detecting the mechanical oscillation of the tip, the device topography, and the Landau levels in the quantum Hall regime at liquid helium temperature and milli-Kelvin temperature.

Transport Properties of Wide Band Gap Semiconductors Louis Tirino III 155 pages Directed by Dr. Kevin F. Brennan The objective of this research has been the study of the transport properties and breakdown characteristics of wide band gap semiconductor materials and their implications on device performance. Though the wide band gap semiconductors have great potential for a host of device applications, many gaps remain in the collective understanding about their properties, frustrating the evaluation of devices made from these materials. The model chosen for this study is based on semiclassical transport theory as described by the Boltzmann Transport Equation. The calculations are performed using an ensemble Monte Carlo simulation method. The simulator includes realistic, numerical energy band structures derived from an empirical pseudo-potential method. The carrier-phonon scattering rates and impact ionization transition rates are numerically evaluated from the electronic band structure. Several materials systems are discussed and compared. The temperature-dependent, high-field transport properties of electrons in gallium arsenide, zincblende gallium nitride, and cubic-phase silicon carbide are compared. Since hole transport is important in certain devices, the simulator is designed to simulate electrons and holes simultaneously. The bipolar simulator is demonstrated in the study of the multiplication region of gallium nitride avalanche photodiodes.

In dieser Arbeit werden Messungen der elektrischen und thermischen Transportkoeffizienten an einem antiferromagnetisch ordnenden Iridat und FeAs-basierten Hochtemperatursupraleitern vorgestellt und analysiert. Iridate sind Materialien mit starker Spin-Bahn-Kopplung. In dem zweidimensionalen Vertreter Sr_2IrO_4 führt diese Kopplung zu isolierendem Mott-Verhalten mit gleichzeitiger antiferromagnetischer Ordnung der gekoppelten Spin-Bahn-Momente. Somit stellt Sr2IrO4 ein Modellsystem für die Untersuchung magnetischer Anregungen dieser Momente in Iridaten dar. Die Analyse der Wärmeleitfähigkeit von Sr_2IrO_4 liefert erstmals klare Hinweise auf magnetische Wärmeleitung in den Iridaten. Die extrahierte magnetische freie Weglänge gibt Aufschluss über die Streuprozesse der zum Wärmetransport beitragenden Magnonen und lässt Schlüsse über die Anregungen des gekoppelten Spin-Bahnsystems zu. Die FeAs-Hochtemperatursupraleiter haben aufgrund ihrer geschichteten Kristallstruktur einen hauptsächlich zweidimensionalen Ladungstransport. Die Phasendiagramme dieser Materialien setzen sich aus Ordnungsphänomenen zusammen, die Magnetismus, Supraleitung und eine Strukturverzerrung umfassen. Das Hauptaugenmerk richtet sich auf die Reaktion der Transportkoeffizienten mit den sich ausbildenden Phasen in Vertretern der 111- und 122-Familien unter chemischer Dotierung innerhalb und außerhalb der Schichtstruktur. Mithilfe von Widerstand und magnetischer Suszeptibilität lassen sich Phasendiagramme der verschiedenen Supraleiterfamilien konstruieren. In ausgewählten Fällen werden der Hall-Koeffizient und elektrothermische Transporteffekte genutzt, um das Phasendiagramm näher zu erforschen. Der Großteil der Untersuchungen zeigt omnipräsente elektrische Ordnungsphänomene, die als nematische Phase bezeichnet werden. Die Messdaten zeigen, dass die Wärmeleitfähigkeit und der Nernst-Koeffizient dominant von Fluktuationen, die der nematischen Phase vorausgehen, beeinflusst werden. Aus den Ergebnissen der Nernst-Daten an dotiertem BaFe_2As_2 werden Schlüsse über die der nematischen Phase zugrunde liegenden Mechanismen des korrelierten Elektronensystems gezogen.

Abstract Carbon nanotubes (CNTs) have fascinating mechanical, electrical and thermal properties, all of which significantly depend on structural properties such as nanotube length, number of walls, lattice defect densities, impurities and surface functional groups. A number of different applications of carbon nanotubes have been demonstrated during the past two decades including electrical interconnects, transistors, heating and cooling devices, sensors and various actuators. However, further studies on the structure-dependent properties and innovative handling techniques of these materials are needed in order to explore the limitations of use and to be able fully to exploit the advantageous properties of such one-dimensional sp2 hybridized carbon nanomaterials. In this thesis, random networks of single-wall and multi-walled carbon nanotubes (SWCNTs and MWCNTs, respectively) and aligned films of multi-walled carbon nanotubes are studied in the context of three main application fields: gas sensing, electrical interconnects/electrodes and thermal cooling elements. Analyses of associated material properties and some feasible integration techniques are discussed. Single-wall and multi-walled carbon nanotube films cast from aqueous dispersions are shown to be selective nitric oxide sensing components in Taguchi-type sensor devices, in which films based on SWCNTs outperformed those made of MWCNTs. The thickness dependent electrical conduction mechanism of inkjet-printed SWCNT films is also discussed. Robust aligned MWCNT films are demonstrated as soft electrical contact brushes in DC motors and in other moving electrical contacts. The thermal properties of freestanding aligned MWCNT forests are analyzed and shown to be potential alternatives to copper or aluminium in the thermal management of electrical components. / Tiivistelmä Hiilinanoputkien kiehtovat mekaaniset, sähköiset ja lämmönjohto-ominaisuudet ovat kiinnostaneet tutkijoita suuresti viimeisten kahden vuosikymmenen ajan. Monia erilaisia applikaatioita on demonstroitu tänä aikana: mukaan lukien sähköiset kontaktit, transistori-rakenteet, lämmitys- ja jäähdytyslaitteet, anturirakenteet sekä erilaiset aktuaattori-rakenteet. Tämän väitöskirjan päätavoitteena on tutkia hiilinanoputkien toiminnollisuutta ja käytännöllisyyttä erilaisissa sovelluskohteissa. Tässä työssä käytettävät hiilinanoputkirakenteet ovat joko satunnaisjärjestyksessä olevia nanoputkista koostuvia verkostorakenteita tai yhdensuuntaisia, makroskooppisia hiilinanoputkikalvoja. Nanoputkia tutkitaan kolmessa erityyppisessä sovelluskohteessa: kaasuanturisovelluksessa, sähköisissä kontaktirakenteissa sekä jäähdytyselementteinä. Työssä analysoidaan hiilinanoputkirakenteiden ominaisuuksia eri sovelluskohteissa sekä esitetään joitain käyttökelpoisia tekniikoita hiilinanoputkien integroimiseen olemassa oleviin tekniikoihin. Hiilinanoputkien osoitetaan olevan käyttökelpoisia aktiivisia materiaaleja typpioksidille resistiivisessä kaasuanturirakenteessa. Tulosten perusteella yksiseinämäiset hiilinanoputket ovat moniseinämäisiä herkempiä ja parempia kyseisessä sovelluksessa. Lisäksi tutkitaan ja analysoidaan mustesuihku-tulostettujen yksiseinämäisten hiilinanoputkifilmien sähköisten ominaisuuksien riippuvuutta filmin paksuudesta. Vantterien yhdensuuntaisten moniseinämäisten hiilinanoputkirakenteiden osoitetaan toimivan erinomaisesti pehmeinä sähköisinä kontaktielementteinä liikkuvissa sähköisissä kontakteissa. Vapaasti seisovien yhdensuuntaisten, moniseinämäisten hiilinanoputkirakenteiden lämmönjohto-ominaisuuksien tutkiminen ja analysointi osoittaa, että kyseisiä rakenteita voidaan käyttää tehokkaina jäähdytyselementteinä ja mahdollisesti korvaavana vaihtoehtona alumiinille ja kuparille sähköisten komponenttien lämmönhallinta sovelluksissa.

This thesis is organized in to six chapters. The contents of each chapter are briefly summarized in the following sections. Chapter 1 introduces different Fe-based superconductors. Within a very short span of their discovery, they quickly expanded to include six different crystal structures. The crystal structure of these systems and their Tc’s are discussed in this chapter. In particular, the properties of Fe1+yTe are described with specific reference to isovalent doping and nonisovalent doping using different elements that affect the superconducting transition in this material. In chapter 2, the basic principles of growth and characterization techniques are explained. These are: 1. Modified Bridgman technique, 2. X-ray diffraction technique, 3. Electron Probe Micro Analyzer to determine chemical composition, 4. SQuID – For magnetization measurements, 5. Closed cycle refrigerator and He Cryostat – for resistivity measurements. The fabrication of high temperature furnace for Bridgman setup is also discussed. Crystal growth and characterization of parent Fe1+yTe and Sb doped Fe1+yTe system are discussed in chapter 3 and chapter 4 respectively. Details of crystal growth by modified Bridgman technique are described here. The characterization includes analysis of crystalline phase, structure and composition. Detailed structural information is extracted from Rietveld refinement of X-ray powder diffraction and the composition analyzed using EPMA. Temperature dependence of magnetization and transport behavior are also discussed. The ideal doping range of Sb in Fe1+yTe is defined in this chapter. In chapter 5, the effect of Sb doping of Fe1.05Te0.50Se0.50 is investigated. The crystal growth and characterization of the new superconductor, Fe1.05Te0.50Se0.48Sb0.02 are deliberated. The superconducting transition observed in transport measurements at zero field and the magnetic field dependence of transition temperatures are discussed. Estimation of upper critical Page|vi|Preface field using Ginzburg-Landau theory as well as the field dependence of magnetization of this crystal is explained in this chapter. The thesis concludes with a chapter on summary and outlook on all investigations. Finally, the scope of future work is outlined in the last section.

In this thesis, synthesis, characterization and electrical transport of Carbon nanotubes (CNTs) have been discussed. The first chapter contains a brief introduction of various forms of carbon including CNT. The CNTs are currently the materials of intense research interest due to their remarkable mechanical and electrical properties. CNTs can be visualized as a graphene sheet that has been rolled into a seamless tube. CNTs are either single-walled carbon nanotubes (SWCNT) or multi-walled carbon nanotubes (MWCNT). SWCNT is a tube with only one wall and MWCNT has many coaxial tubes and weak Van der Waal forces hold them together. The properties depend on chirality, diameter and length of the tubes. Chirality is defined by the symmetry and the chiral angle formed between the carbon bonds. The atomic structure of CNTs is described in terms of the tube chirality, which is defined by the chiral vector Ch and the chiral angle . The chiral vector is Ch = na1 + ma2, where the integers (n, m) are the number of steps along the zig-zag carbon. Depending on the tube chirality the electrical properties of the CNTs differ; they can be metallic or semiconducting. When n-m = 3p, where p is an integer, the CNTs are metallic and when n-m  3p, the CNTs are semiconducting. Due to the high anisotropy and high aspect ratio, CNTs have many potential applications with great technological importance such as functionalized molecules, conductive wires, bearings of rotational motors, field emitters, hydrogen storage, sensors, polymer composites, nanotube yarn and nanotube filters, X-ray generator, electron sources for microscopy and lithography, gas discharge tubes and vacuum microwave amplifiers, etc. The first chapter gives a brief introduction about various forms of carbon and their properties, particularly of CNTs. The nature of the CNTs depends on the method of production, which controls the degree of graphitization, the tube diameter and the chirality. Most synthesis methods originate from the idea of obtaining adequately active carbon atomic species or clusters from carbon sources and assembling them into CNTs without or with catalysts. The commonly used methods for the synthesis of carbon nanotubes are arc-discharge, Laser ablation, high-pressure catalytic decomposition of carbon monoxide (HiPCO), electrophoretic deposition (EPD), flame synthesis, pyrolysis, chemical vapour deposition (CVD), hot-filament CVD, plasma enhanced chemical vapour deposition (PECVD) using DC, RF, and micro wave power sources, hot-filament dc (HF-dc PECVD), inductively coupled plasma (ICPECVD) and electron cyclotron resonance (ECR PECVD). Although many efforts have been made to develop various synthesis methods, most of them require many steps. Moreover, the complicated and rigorous control of parameters and expensive materials are unavoidable that has put limitation in reproducing the same in large scale. In this chapter, a simple method for the synthesis of CNTs on a large scale that eliminates nearly the entire complex and expensive machinery associated with widely used growth techniques has been discussed. In Chapter 2, the synthesis and characterization of entangled CNTs are discussed. It is shown that entangled CNTs can be synthesized in one step by using double stage furnace. Tetrahydrofuran as carbon source material and nickelocene as catalyst source material have been used to synthesize CNTs. With this method CNTs can be synthesized at a temperature as low as at 600 0C. In this technique the self-developed pressure carries the vapours to the hot zone of the furnace. This has led to think in modifying the double stage furnace. A single stage furnace having temperature gradient is made to synthesize CNTs. The vapours are carried from low temperature zone to hot zone where the carbon species and catalysts react to form CNTs. The advantage of this furnace is that it is one-step process. Using another carbon source material such as Diethyl Ether and nickelocene as catalyst source material CNTs are synthesized. The as synthesized and purified CNTs are characterized by X-ray diffraction (XRD), Scanning electron microscope (SEM), transmission electron microscope (TEM), high resolution TEM (HRTEM) and Raman spectroscopy. The CNTs are multi-walled in nature as observed by HRTEM. In Chapter 3, the synthesis of aligned CNTs is discussed by using benzene as carbon source and ferrocene as catalyst source materials. Aligned MWCNTs were synthesized in the temperature range between 650 - 1100 0C in a single stage furnace without the need for carrier gas nor predeposited metal catalyst substrate. The essential need of CNTs are (1) to obtain aligned nanotubes with millimeter lengths to enable the formation of novel nanotube-polymer composites that incorporate continuous nanotubes throughout their thickness for highly anisotropic thermal and electrical conductivities; and (2) to provide samples for detailed physical characterization - tensile strength, thermal, electrical conductivity, field emission etc. SEM observation reveals the increase in length of nanotubes from 85 m to 1.4 mm with the increase of preparation temperature. The diameter as investigated by high-resolution transmission electron microscopy (HRTEM) remains almost constant 70-80 nm (75-85 layers). Once nanotube formation is established, the growth continues in the same direction and may well be reinforced by the presence of surrounding CNTs i.e. almost every particle produces a nanotube and bundling of neighboring tubes lead to collective vertical growth. The increase in length is due to the enhanced diffusion of active carbon with increasing preparation temperatures. The alignment of CNTs is also observed to the lateral side of the substrate. In Chapter 4, the synthesis and characterization of carbon nanoribbon and singled crystal iron filled CNTs is discussed. Particularly interesting are those CNTs filled with magnetic nanowires, which can provide an effective barrier against oxidation and consequently ensure a long-term stability in the core. The filling of metals within carbon nanotubes has extended the potential application base of these materials to quantum memory elements, high density magnetic storage media, semiconducting devices, field electron emitters, high resolution magnetic atomic force microscopy tips, magnetic field sensors and scanning probe microscopes etc. Tetrahydrofuran as carbon source material and ferrocene as catalyst materials has been used to synthesize mixture of carbon nanoribbons and iron filled CNTs. The techniques used to characterize the materials are XRD, SEM, HRTEM and superconducting quantum interference device (SQUID). The powder XRD pattern shows that the bcc -Fe phase of iron is present. HRTEM studies reveal the presence of multi-walled carbon nanotubes and well-crystallized -Fe phase filled inside the core region. Closer inspection of the HRTEM images indicated that the bcc structure -Fe nanowires are monocrystalline and Fe (110) plane is indeed perpendicular to the G (002) plane. Large coercivity (i.e. 1037 Oe at 300 K and 2023 Oe at 10 K) in the iron filled CNTs and carbon nanoribbons have been observed. The high coercivity is mainly attributed to the following two factors. Firstly, it is known that due to the uniaxial magnetic anisotropy of the nano size iron in the core region of the carbon nanotubes. Secondly, ferromagnetic behavior exhibited by the localized states at the edges of the carbon nanoribbons. The anisotropic electrical transport property of MWCNTs has been discussed in the chapter 5. The activated diffusive nature of transport along axial direction of CNT is explained. The transport perpendicular to the tube direction is explained in terms of a hopping mechanism. The anisotropic resistivity (N/P) value obtained is 3. The temperature dependent magnetoresistance (MR) is studied in magnetic fields up to 11 Tesla at low temperatures both in the parallel and perpendicular direction of an aligned MWCNT mat. In both cases a negative MR is observed. Chapter 6 discusses the preparation of CNT-polymer composites. The temperature dependence of the conductivity and magnetoresistance (MR) has been studied making four-point contact method on the carbon nanotubes polymer composites as result of increasing CNT content. The conductivity increases with increasing carbon nanotube weight percentage. The increase in conductivity as a function of the CNT weight percent is attributed to the introduction of conducting CNT paths in the polymer matrix. With the increasing CNT content the number of interconnections present in a random system is found to vary. Electrical conduction in nanotube mat or nanotube composites is explained by a variable range hopping (VRH) conduction mechanism. The negative magnetoresistance has been observed for the polymer composites. It is consistent with the report on CNTs bundles and polymer composites. Finally a brief summary of the work presented in this dissertation is discussed along with future directions in this research.

Orientador: Luis Vicente de Andrade Scalvi / Resumo: Este trabalho visa apresentar o desenvolvimento e as principais conclusões referentes à combinação de heterojunções a base de GaAs com óxidos semicondutores, para aplicações em dispositivos optoeletrônicos. O texto foi dividido em duas partes principais, sendo a primeira parte voltada para a síntese e produção do SnO2, relacionada com a formação da heteroestrutura GaAs/SnO2; e a segunda parte é focada na produção dos ressonadores de onda acústicas de bulk,na ordem de GHz, a base de GaAs/ZnO. Na primeira parte, priorizou-se filmes de SnO2, que foram depositados por duas técnicas: sol-gel dip-coating e evaporação resistiva. Os filmes foram depositados sobre substratos de vidro soda-lime, e sobre substratos de GaAs, de quartzo e de a-SiO2. SnO2 foi também depositado sobre filme de GaAs depositado por sputtering. No caso da evaporação resistiva, a rota sol-gel é utilizada também para a preparação do pó que é utilizado como precursor para a evaporação resistiva de filmes de SnO2, combinando essas duas técnicas. Foram investigadas as propriedades ópticas e elétricas de filmes finos de SnO2 dopado com 1% de Er3+ e estruturas hibridas de GaAs/SnO2: Er3+. Entre os principais resultados, verificou-se: 1) espectros de luminescência diferentes do íon Er3+ ao se depositar SnO2 sobre substrato de vidro ou GaAs; 2) Microscopia eletrônica de varredura (MEV) e espectroscopia de energia dispersiva de raios-x (EDX) para filmes de SnO2, depositados por evaporação resistiva, atestaram uma relação... (Resumo completo, clicar acesso eletrônico abaixo) / Abstract: This work aims to present the development and the main conclusions obtained so far regarding the combination of GaAs-based heterojunctions with semiconductor oxides, for applications in optoelectronic devices. The text has been divided in two main parts, where the first one is related to the synthesis and production of SnO2, associated with the formation of the heterostructure GaAs/SnO2; and the second one if focused on the production of bulk acoustic wave resonators, with frequencies in GHz range, based on GaAs/ZnO. In the first part, attention was given to SnO2 films, deposited by two techniques: sol-gel dipcoating and resistive evaporation, on soda-lime glass substrates, and on GaAs, quartz and a-SiO2 substrates. SnO2 was also deposited on GaAs film deposited by sputtering. In the case of resistive evaporation, the sol-gel route is also used to prepare the powder which is used as a precursor for resistive evaporation of SnO2 films, then, by combining these two techniques. Optical and electrical properties of Er3+ -doped SnO2 thin films were investigated as well as the hybrid structure GaAs/SnO2 .Among the main results were: 1) different luminescence spectra of Er3+ ion when depositing SnO2 on glass or GaAs substrate; 2) scanning electron microscopy (SEM) and energy dispersive x-ray spectroscopy (EDX) for SnO2 films deposited by resistive evaporation show a relationship of the thermal annealing temperature with the concentration of Er ions in the surface layers; 3) this con... (Complete abstract click electronic access below) / Doutor