Theoretical predictions of the AC conductivity of both monolayer and Bernal-stacked bilayer graphene have largely been in agreement with experimental observations. Due to the recent realization of AA-stacked samples, we provide theoretical predictions for this system. We begin this thesis with a review of the optical properties of graphene and provide a brief discussion of the previously studied Bernal-stacked bilayer. We then calculate the optical conductivity of AA-stacked bilayer graphene as a function of frequency for several interesting cases. We are primarily interested in the case of finite doping due to charging. Unlike the monolayer, we see a Drude absorption at charge neutrality as well as an interband absorption with strength twice that of the monolayer background conductivity which onsets at twice the interlayer hopping energy. We examine the behaviour as we vary the chemical potential relative to the interlayer hopping energy scale and compute the partial optical sum. We also consider the effect of adding a bias across the layers and find it serves merely to renormalize the interlayer hopping parameter. While interested in the in-plane conductivity we also provide the perpendicular conductivity of the AA-stacked bilayer. We then extend the ideas to the AAA-stacked trilayer. Based on proposed models for topological insulators discussed in the literature, we consider the effect of spin orbit coupling in both one and two layers on the optical properties of the AA-stacked bilayer which illustrates the effect of opening an energy gap in the band structure.

Graphene is one of the most popular material due to its promising properties, for instance electronics applications. Graphene films were grown on silicon carbide (SiC) substrate using chemical vapor deposition (CVD). Influence of the deposition temperature on the morphology of the films was investigated. Characterizations were done by reflectance mapping, atomic force microscopy and Raman spectroscopy. Two samples were done by sublimation process, to compare the number of layers and the morphology of the graphene films with the one grown by chemical vapor deposition.The reflectance mapping showed that the number of layers on the samples made by CVD was notinfluenced by the deposition temperature. But also, demonstrated that sublimation growth is present in allthe samples due to the presence of silicon coating in the susceptor. The growth probably started by sublimation and then CVD deposition. The step morphology characteristic of the silicon carbide substrate surface was conserved during the deposition of graphene. But due to surface step bunching, a decrease inthe step height occurred and the width of the terraces increased. The decreasing in deposition temperature leads to a smoother surface with the CVD method. Raman spectroscopy confirmed the presence ofgraphene and of the buffer layer characteristic of the sublimation growth. Moreover, it demonstrated the presence of compressive strain in the graphene layers.

As an atomic layer of sp2-hybridized carbon atoms closely packed in a honeycomb lattice, graphene has been attracting increasing attention since its discovery in 2004 due to its extraordinary physicochemical properties. Graphene oxide (GO), a non-stoichiometric graphene derivative with the carbon plane abundantly decorated with hydroxyl, epoxide and carboxylic groups, can be massively and cost-effectively produced from natural graphite following Hummers method. GO has greater aqueous solubility than pristine graphene due to its oxygen-functionalities. Various solution-based chemical methods can be applied to GO, which has stimulated a new research area called ???wet chemistry of grahene???. Among them, chemical reduction of GO provides a facile route for large-scale synthesis of graphene. With abundant oxygen-functionalities in its structure, GO can potentially act as a suitable precursor for chemical modifications of graphene through methods used in organic chemistry. Special attention should be paid to that the hydroxyl groups in GO belong to tertiary alcohols, and steric hindrance should be considered when performing chemical modifications. Diethylaminosulfur trifluoride (DAST), a fluorinating reagent, is ineffective in fluorinating GO due to the steric hindrance of tertiary hydroxyls. However, DAST is effective in reducing GO. The capability of DAST for GO reduction is close to hydrazine, but the reduction reaction can be performed at lower temperature for DAST. As a two-dimensional (2D) nanomaterial with good aqueous solubility, biocompatibility and excellent intrinsic mechanical properties, GO is particularly useful in preparing 3D hybrid hydrogel scaffolds for tissue engineering applications.

Three dimensional (3D) hybrid architectures are new types of materials that have a number of technological applications. However, the synthesis of such materials has been problematic to date. The objective of this study is to fabricate 3D hybrid architectures composed of sp2-carbon nanomaterials and inorganic nanostructures using a convenient microwave assisted technique. Sp2-Carbon nanomaterials such as carbon nanotubes (CNTs), graphene and its derivative graphene oxide (GO), have been explored by researchers as major components of hybrid materials due to their exceptional electrical, thermal, mechanical and biological properties. However, most of the research has been devoted to the hybrids with randomly dispersed phases. The present study explores the feasibility of using aligned 3D sp2-carbon structures in a bottom-up microwave-assisted chemical synthesis approach to fabricate various 3D sp2-carbon/inorganic hybrid architectures. The carbon nanostructures, either tubular or planar, not only contribute to the functionalities of the hybrids, but also template the ordered assembly of phases on nanometer scale. Mimicking nature is a key to develop novel types of materials with enhanced physical and mechanical properties suitable for advanced applications (e.g. lightweight and yet tough materials that are extensively needed in automotive and aerospace industries). One approach to obtain such materials or devices is to mimic nature processes and synthesize hybrid materials with ordered structures on the nanometer scale. Those functional structures are fabricated in this thesis through an in-situ microwave synthesis of inorganic materials on 3D sp2-carbon architectures. Generally, in chapter 1, it was shown and discussed the procedures to fabricate 3D architectures of carbon nanotubes and graphene oxide as basic components for template synthesis of the hybrids. Then in chapter 2 the microwave chemical synthesis approach was introduced as a convenient route for fabricating inorganic materials such as zinc oxide (ZnO) which was shown to be used as UV sensors. Through photolithography patterning of the iron catalyst thin films on Si/SiO2 substrates, 3D aligned CNT structures were fabricated and were coated in-situ with inorganic materials such as cobalt oxide, zinc oxide and manganese oxide using a microwave synthesis approach (chapter 3). The obtained aligned strips of CNT/Co3O4 were chosen as an example to illustrate the application of such 3D hybrids in energy storage applications. The capacitance of the aligned CNT/Co3O4 strips was measured to be 123.94 F/g. Using graphene oxide as template for manufacturing the 3D sp2-carbon/inorganic hybrid structures, interesting novel layered configurations are obtained that are similar to the layered structures of exoskeleton of the mollusks nacre. The layered hybrid structure shown to be mechanically improved compared to its constituents (chapter 4). Finally in chapter 5, some of the future routes have been proposed for further research on this novel field of 3D hybrid materials composed of sp2-carbons and inorganic nanomaterials.

Nanotechnology is providing a new set of tools to the engineering community to design nanoscale components with unprecedented functionalities. The integration of several nano-components into a single entity will enable the development of advanced nanomachines. Nanonetworks, i.e., networks of nanomachines, will enable a plethora of applications in the biomedical, environmental, industrial and military fields. To date, it is still not clear how nanomachines will communicate. The miniaturization of a classical antenna to meet the size requirements of nanomachines would impose the use of very high radiation frequencies. The available transmission bandwidth increases with the antenna resonant frequency, but so does the propagation loss. Due to the expectedly very limited power of nanomachines, the feasibility of nanonetworks would be compromised if this approach were followed. Therefore, a new wireless technology is needed to enable this paradigm. The objective of this thesis is to establish the foundations of graphene-enabled electromagnetic communication in nanonetworks. First, novel graphene-based plasmonic nano-antennas are proposed, modeled and analyzed. The obtained results point to the Terahertz Band (0.1-10 THz) as the frequency range of operation of novel nano-antennas. For this, the second contribution in this thesis is the development of a novel channel model for Terahertz Band communication. In addition, the channel capacity of the Terahertz Band is numerically investigated to highlight the potential of this still-unregulated frequency band. Third, a novel modulation based on the transmission of femtosecond-long pulses is proposed and its performance is analyzed.% in terms of achievable information rates. Fourth, the use of low-weight codes to prevent channel errors in nanonetworks is proposed and investigated. Fifth, a novel symbol detection scheme at the receiver is developed to support the proposed modulation scheme. Sixth, a new energy model for self-powered nanomachines with piezoelectric nano-generators is developed. Moreover, a new Medium Access Control protocol tailored to the Terahertz Band is developed. Finally, a one-to-one nano-link is emulated to validate the proposed solutions.

Graphene, the two-dimensional lattice of sp2-hybridized carbon atoms, has a great potential for future electronics, in particular for opto-electronic devices. The carrier relaxation dynamics, which is of key importance for such applications, is in the main focus of this thesis. Besides a short introduction into the most prominent material properties of graphene and the experimental techniques, this thesis is divided into three main parts. The investigation of the carrier relaxation dynamics in the absence of a magnetic field is presented in Chapter 3. In the first experiment, the anisotropy of the carrier excitation and relaxation in momentum space was investigated by pump-probe measurements in the near-infrared range. While this anisotropy was not considered in all previous experiments, our measurements with a temporal resolution of less than 50 fs revealed the polarization dependence of the carrier excitation and the subsequent relaxation. About 150 fs after the electrons are excited, the carrier distribution in momentum space gets isotropic, caused by electron-phonon scattering. In a second set of two-color pump-probe experiments, the temperature of the hot carrier distribution, which was obtained within the duration of the pump pulse (about 200 fs), could be estimated. Furthermore, a change in sign of the pump-probe signal can be used as an indicator for the Fermi energy of different graphene layers. Pump-probe experiments in the far-infrared range in reflection and transmission geometry were performed at high pump power. A strong saturation of the pump-induced transmission was found in previous experiments, which was attributed to the pump-induced change in absorption. Our investigation shows the strong influence of pump-induced reflection at long wavelengths, as well as a lot smaller influence of the saturation of the pump-induced change in absorption. At a high pump power, the increase of the reflection exceeds the change in absorption strongly, which leads to negative pump-probe signals in transmission geometry. In Chapter 4, investigations of the carrier dynamics of graphene in magnetic fields of up to 7T are presented. Even though the optical properties of Landau-quantized graphene are very interesting, the carrier dynamics were nearly unexplored. A low photon energy of 14meV allows the investigation of the intraband Landau-level (LL) transitions. These experiments revealed two main findings: Firstly, the Landau quantization strongly suppresses the carrier relaxation via optical-phonon scattering, resulting in an increased relaxation time. Secondly, a change in sign of the pump-probe signal can be observed when the magnetic field is varied. This change in sign indicates a hot carrier distribution shortly after the pump pulse, which means that carrier-carrier scattering remains very strong in magnetic fields. In a second set of pump-probe measurements, carried out at a photon energy of 75meV, the relaxation dynamics of interband LL transitions was investigated. In particular, experiments on the two energetically degenerate LL transitions LL(−1)->LL(0) and LL(0)->LL(1) showed the influence of extremely strong Auger processes. An ultrafast and extremely broadband terahertz detector, based on a graphene flake, is presented in the last chapter of this thesis. To couple the radiation efficiently to the small flake, the inner part of a logarithmic periodic antenna is connected to it. With a rise time of about 50 ps in a wavelength range of 9 μm to 500 μm, this detector is very interesting to obtain the temporal overlap in two-color pump-probe experiments with the free-electron laser FELBE. Furthermore, the importance of the substrate material, in particular for the high-speed performance, is discussed.

Because of its high theoretical specific capacity (4200mAh/g) and natural abundance (2nd most abundant element on earth), silicon is considered a promising anode candidate for high energy density lithium-ion batteries. However, the dramatic volume changes (up to 400%) that occur during lithiation/delithiation and the relative low electrical conductivity of silicon prevent the implementation of this material. In this work, a nano-silicon/polyaniline/reduced graphene oxide composite was synthesized via a two-step process: in-situ polymerization of polyaniline (PANi) in the presence of nano-silicon followed by combination of the prepared n-Si/PANi binary composite with reduced graphene oxide (RGO), to form a n-Si/PANi/RGO composite. Electron microscopy reveals the unique nano-architecture of the n-Si/PANi/RGO composite: silicon nanoparticles are well dispersed within a PANi matrix, which in turn is anchored to the surface of RGO sheets. The n-Si/PANi/RGO ternary composite delivered an initial capacity of 3259 mAh/g and 83.5% Coulombic efficiency. The new composite displayed better rate performance and capacity recovery than either nano-Si or n-Si/PANi. Structural and morphological studies combined with AC impedance analysis suggest that the n-Si/PANi/RGO composite has higher electrical conductivity than the other two component materials, yielding better performance at high current densities or C rates. The good rate performance, high initial specific capacity and stable Coulombic efficiency of n-Si/PANi/RGO make it a promising anode material for high energy density lithium-ion batteries.

Because of its high theoretical specific capacity (4200mAh/g) and natural abundance (2nd most abundant element on earth), silicon is considered a promising anode candidate for high energy density lithium-ion batteries. However, the dramatic volume changes (up to 400%) that occur during lithiation/delithiation and the relative low electrical conductivity of silicon prevent the implementation of this material. In this work, a nano-silicon/polyaniline/reduced graphene oxide composite was synthesized via a two-step process: in-situ polymerization of polyaniline (PANi) in the presence of nano-silicon followed by combination of the prepared n-Si/PANi binary composite with reduced graphene oxide (RGO), to form a n-Si/PANi/RGO composite. Electron microscopy reveals the unique nano-architecture of the n-Si/PANi/RGO composite: silicon nanoparticles are well dispersed within a PANi matrix, which in turn is anchored to the surface of RGO sheets. The n-Si/PANi/RGO ternary composite delivered an initial capacity of 3259 mAh/g and 83.5% Coulombic efficiency. The new composite displayed better rate performance and capacity recovery than either nano-Si or n-Si/PANi. Structural and morphological studies combined with AC impedance analysis suggest that the n-Si/PANi/RGO composite has higher electrical conductivity than the other two component materials, yielding better performance at high current densities or C rates. The good rate performance, high initial specific capacity and stable Coulombic efficiency of n-Si/PANi/RGO make it a promising anode material for high energy density lithium-ion batteries.

This thesis presents the theoretical studies of electronic transport in molecular electronic devices. Such devices have been proposed and investigated as a promising new approach that complements conventional silicon-based electronics. To design and fabricate future nanoelectronic devices, it is essential to understand the conduction mechanism at a molecular or atomic level. Our approach is based on the non-equilibrium Green's function method (NEGF) combined with density functional theory (DFT). We apply the method to study the electronic transport properties of two-probe systems consisting of molecules or atomic wires sandwiched between leads. A few molecular electronic devices are characterized; namely, conducting molecular wires, molecular switches and molecular recognition sensors. The considered applications are interconnection of different nanoelectronic units with cumulene molecular wires; adding switching functionality to the molecular connectors by applying stress to the CNT-cumulene-CNT junction or by introducing phthalocyanine unit; sensing of individual nucleotides, e.g., for DNA sequencing applications. The obtained results provide useful insights into the electron transport properties of molecules. Several interesting and significant features are analyzed and explained in particular such as, level pinning, negative differential resistance, interfering of conducting channels etc.

A large family of materials, collectively known as "van der Waals materials," have attracted enormous research attention over the past decade following the realization that they could be isolated into individual crystalline monolayers, with charge carriers behaving effectively two-dimensionally. More recently, an even larger class of composite materials has been realized, made possible by combining the isolated atomic layers of different materials into "van der Waals heterostructures," which can exhibit electronic and optical behaviors not observed in the parent materials alone. This thesis describes efforts to characterize the atomic-scale structural and electronic properties of these van der Waals materials and heterostructures through scanning tunneling microscopy measurements. The majority of this work addresses the properties of monolayer and few-layer graphene, whose charge carriers are described by massless and massive chiral Dirac Hamiltonians, respectively. In heterostructures with hexagonal boron nitride, an insulating isomorph of graphene, we observe electronic interference patterns between the two materials which depend on their relative rotation. As a result, replica Dirac cones are formed in the valence and conduction bands of graphene, with their energy tuned by the rotation. Further, we are able to dynamically drag the graphene lattice in these heterostructures, owing to an interaction between the scanning probe tip and the domain walls formed by the electronic interference pattern. Similar dragging is observed in domain walls of trilayer graphene, whose electronic properties are found to depend on the stacking configuration of the three layers. Scanning tunneling spectroscopy provides a direct method for visualizing the scattering pathways of electrons in these materials. By analyzing the scattering, we can directly infer properties of the band structures and local environments of these heterostructures. In bilayer graphene, we map the electrically field-tunable band gap and extract electronic hopping parameters. In WSe₂, a semiconducting transition metal dichalcogenide, we observe spin and layer polarizations of the charge carriers, representing a coupling of the spin, valley and layer degrees of freedom.