Self-assembly of nanomaterials over macroscopic dimensions and development of novel nano-electromechanical systems (NEMS) hold great promise for numerous nanotech applications. However, it has always been a great challenge to find a general route for controlled self-assembly of nanomaterials and generating electromechanical response at the nanoscale level. This work indicates that self-organized anisotropic nematic liquid crystals (LC) can be exploited for nanotemplating purposes to pattern carbon nanotubes (CNTs) and Quantum dots (QDs) over a macroscopic dimension. The pattern formed by the CNTs or QDs can be controlled by applying external electric and magnetic fields, developing novel nano-electromechanical and nano-magnetomechanical systems. Self-organizing nematic liquid crystals (LC) impart their orientational order onto dispersed carbon nanotubes (CNTs) and obtain CNT-self-assembly on a macroscopic dimension. The nanotubes-long axis, being coupled to the nematic director, enables orientational manipulation via the LC nematic reorientation. Electric field induced director rotation of a nematic LC+CNT system is of potential interest due to its possible application as a nano-electromechanical system. Electric field and temperature dependence of dielectric properties of an LC+CNT composite system have been investigated to understand the principles governing CNT-assembly mediated by the LC. In the LC+CNT nematic phase, the dielectric relaxation on removing the applied field follows a single exponential decay, exhibiting a faster decay response than the pure LC above a threshold field. Due to a strong LC-CNT anchoring energy and structural symmetry matching, CNT long axis follows the director field, possessing enhanced dielectric anisotropy of the LC media. This strong anchoring energy stabilizes local pseudo-nematic domains, resulting in nonzero dielectric anisotropy in the isotropic LC phase. These anisotropic domains respond to external electric fields and show intrinsic frequency response. The presence of these domains makes the isotropic phase electric field-responsive, giving rise to a large dielectric hysteresis effect. These polarized domains maintain local directors, and do not relax back to the original state on switching the field off, showing non-volatile electromechanical memory effect. Assembling quantum dots (QDs) into nanoscale configurations over macroscopic dimensions is an important goal to realizing their electro-optical potential. In this work, we present a detailed study of a pentylcyanobiphenyl liquid crystal (LC) and a CdS QD colloidal dispersion by probing the dielectric property  and relaxation as a function of an applied ac-electric field Eac. In principle, dispersing QDs in a nematic LC medium can direct the dots to align in nearly one-dimensional chain-like structures along the nematic director and these assemblies of QDs can be directed by external electric fields. In a uniform planar aligned cell, the Fréedericksz switching of the LC+QDs appears as a two-step process with the same initial switching field as the bulk but with the final value larger than that for an aligned bulk LC. The relaxation of  immediately following the removal of Eac follows a single-exponential decay to its original value that is slower than the bulk but becomes progressively faster with increasing Eac, eventually saturating. These results suggest that the arrangement of the QDs is mediated by the LC.

Thermoelectric generators are solid state machines used to convert temperature gradients into electrical energy. They are formed by several thermoelectric units connected electrically in series and thermally in parallel. These units are made by creating a junction between a p-type and an n-type conductor. This investigation documents the characterisation of the thermoelectric properties of carbon nanotube (CNT) films and the fabrication process of carbon nanotube-based thermoelectric devices. The Seebeck coefficient is a intrinsic property of a thermoelectric material that correlates the voltage produced by a conductor and the temperature gradient applied to it. To measure the Seebeck coefficient of films, an experimental set-up was fabricated and calibrated using constantan as standard material. CNT films of aligned nanotubes fabricated using a chemical vapour deposition method were analysed. The Seebeck coefficient along and across the samples did not show significant variations, with values between 40$\mu$V/K and 80$\mu$V/K. Using these CNT films, thermoelectric cells were fabricated with the CNT as the p-type conductor and constantan as the n-type. As a proof of concept, two hand-made thermoelectric generators were assembled by connecting hundreds of these thermoelectric cells. These devices were subjected to a temperature gradient of $\approx$200K, which was enough to produce enough power to light an LED. Other analytical techniques were used to characterise the materials used in this work. Electrical conductivity measurements, thermogravimetric analysis, Raman spectroscopy and scanning electron microscopy were performed. Using a deposition technique, films of nanotubes were produced from a liquid phase. The impact of the production method on their properties was evaluated. Characterisation equipment was developed to measure the Seebeck coefficient and thermal conductivity. Thermoelectric devices made with the carbon nanotube films were fabricated and characterised. The values of thermal conductivity of the CNT films analysed in this work are between 0.86Wm$^{-1}$K$^{-1}$. The electrical conductivity of these materials is between 3500Sm$^{-1}$ and 14100Sm$^{-1}$. The maximum figure of merit of the carbon nanotube thermoelectric devices fabricated in this work is $ZT$=0.35.

The main goal of this project was the development of carbon nanotubes as a candidate for dual-functioning magnetic hyperthermia structure and magnetic resonance imaging contrast agent. This was achieved by filling carbon nanotubes with continuous ferromagnetic α-Fe nanowires and surface functionalized with paramagnetic Gd(III). Also, length control of both nanotube and nanowire was investigated. Firstly, a low vapour flow-rate and constant evaporation temperature chemical vapour deposition method based on the thermal decomposition of ferrocene was employed which achieved continuous α-Fe nanowires on the same scale as the nanotube for lengths >10 m without the necessity of post-synthesis heat-treatment or introduction of other precursor elements. The low vapour flow-rate regime has the advantage of sustaining the intrinsic temperature gradient at the tip of the forming structure which drives the vapour feedstock to the growth front to guarantee continuous nanowire formation. For initially mixed-phase nanowires of length less than 10 μm, the continuous α-Fe nanowires were achieved by postsynthesis heat treatment. Secondly, a simple wet chemical method involving only sonication in aqueous GdCl3 solution was used for surface functionalization of iron-filled multiwalled carbon nanotubes with gadolinium. Functional groups on the sidewalls produced by the sonication provide active nucleation sites for the loading of Gd3+ ions. Characterization by electron paramagnetic resonance, electron energy loss spectroscopy, and high-resolution transmission electron microscopy confirmed the presence of Gd3+ ions on the sidewall surface. The ferromagnetic properties of the encapsulated iron nanowire maintained after surface functionalization. At room temperature a saturation magnetization of 40 emu/g and a coercivity of 600 Oe were observed. Heating functionality in an alternating applied magnetic field was quantified through the measurement of specific absorption rate: 50 W/gFe and the intrinsic loss power: 1.12 nHm²kg⁻¹ at magnetic field strength 8 kA/m and frequency of 696 kHz. These structures exhibited an extremely high relaxivity r₁ ~ 200 mM⁻¹ s⁻¹ at high magnetic field (9.4 T).

This thesis describes a detection system for single molecules based on individual single-walled carbon nanotube field-effect sensors. The sensitivity, spatial confinement and transducer gain of the sensor is derived from a conductance controlled electrochemically created defect, which is also chemically reactive. An automated microfluidic system is designed to enable long and stable measurements of the carbon nanotube device in aqueous environment with temperature control of ±0.1°C. A probe DNA can be covalently attached to the defect through an amide bond and the conductance is modulated when a target DNA binds to the probe. As a result, the conductance shows a traditional random telegraph signal and fluctuates between a hybridized and melted state. By monitoring the conductance as a function of temperature, the kinetics and thermodynamics can be extracted, which are comparable to previous fluorescent correlation spectroscopy studies using optical fluorescent resonant energy transfer. By studying the fluctuation amplitude as a function of charge proximity, buffer concentration and solution potential, it is shown that the sensor is based on a field-effect. The sensor has a temporal resolution of 200 μs and a signal to noise ratio of 3-8 when continuously measuring for 30 seconds. By further reducing the parasitics, the sensor has the capabilities to detect biomolecule kinetics down to microsecond resolution, which could make it an attractive tool for single-molecule experiments with fast kinetics.

Coulomb drag-induced ion current flow is reported, achieved through coupling of electronic charge carriers along the lattice of a narrow single-walled carbon nanotube to electrolytic charge within the confines of the nanotube. Solid-state electrical contacts to the nanotube induce ion transport through it in the absence of an axial electric field; in the presence of such a field, the device behaves as an n-type ionic transistor. Ionic currents as high as 1nA have been recorded without alternate driving forces. Asymmetric functionalization of single walled carbon nanotube end groups further enhances the rectifying behavior of the device, yielding a current rectification ratio as high as 10 at moderate axial field strengths. By achieving ion pumping through a solid-state electrical input, the system offers promising solutions to nanoscale applications including purification, drug delivery, and desalination.

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Low-dimensional systems are an important and intensely studied area of condensed matter physics. When a material is forced to adopt a low-dimensional structure, its behaviour is often dramatically different to that of the bulk phase. It is vital to predict the structures of low-dimensional systems in order to reliably predict their properties. To this end, the ab initio random structure searching (AIRSS) method, which has previously been used to identify the structures of bulk materials, has been extended to deal with the case of nanowires encapsulated inside carbon nanotubes. Such systems are a rapidly developing area of research with important nanotechnological applications, including information storage, energy storage and chemical sensing. The extended AIRSS method for encapsulated nanowires (ENWs) was implemented and used to identify the structures formed by germanium telluride, silver chloride, and molybdenum diselenide ENWs. In each of these cases, a number of novel nanowire structures were identified, and a phase diagram predicting the ground state nanowire structure as a function of the radius of the encapsulating nanotube was calculated. In the case of germanium telluride, which is a technologically important phase-change material, the potential use of GeTe ENWs as switchable nanoscale memory devices was investigated. The vibrational properties of silver chloride ENWs were also considered, and a novel scheme was developed to predict the Raman spectra of systems which can be decomposed into multiple weakly interacting subsystems. This scheme was used to obtain a close approximation to the Raman spectra of AgCl ENWs at a fraction of the computational cost that would otherwise be necessary. The encapsulation of AgCl was shown to produce substantial shifts in the Raman spectra of nanotubes, providing an important link with experiment. A method was developed to predict the stress-strain response of an ENW based on a polygonal representation of its surface, and was used to investigate the elastic response of molybdenum diselenide ENWs. This was used to predict stress-radius phase diagrams for MoSe_2 ENWs, and hence to investigate stress-induced phase change within such systems. The X-ray diffraction of ENWs was also considered. A program was written to simulate X-ray diffraction in low-dimensional systems, and was used to predict the diffraction patterns of some of the encapsulated GeTe nanowire structures predicted by AIRSS. By modelling the interactions within a bundle of nanotubes, diffraction patterns for bundles of ENWs were obtained.

Carbon nanotubes and graphene have been a trending research topic in the past decade. These graphitic compounds exhibit numerous advantageous properties (electronic, mechanical, thermal, optical, etc) which industry and researchers alike are excited to take advantage of. Beyond the challenges of yield and controlled growth, there are a number of standing questions which govern some of the more fundamental characteristics of these materials: What role do lattice defects play in the adsorption of gas molecules on the surface of carbon nanotubes? How are the electronic states of the carbon nanotubes influenced by these adsorbed molecules? And how can we develop models to predict useful applications of this knowledge? In order to address these questions, this study combines Raman spectroscopy and electronic measurements carried out in highly controlled environments of carbon nanotube transistors. Assessing these data in conjunction shows that the defect density of a carbon nanotube channel has no correlation with observed threshold voltage shifts, or change in Schottky barrier, due to the presence of ambient oxygen. With these insights in mind, a dynamic adsorption-desorption model is proposed which addresses the oxygen sensitivity of carbon nanotube transistors. Instrumentation and computational developments which facilitated these measurements are also disclosed.