Molybdenum chalcohalide nanowires are systems, which structural, electronic and optical properties have been analyzed in detail. However, their potential as building blocks for electronic devices has not been investigated so far. This question is raised in Dissertation, focusing on unique electronic transport properties of these systems, and comparing them with those of the popular carbon nanotubes.

Having conducted the research described in this thesis I found that there exists a possibility to produce polyelectrolyte nanostructures on hydrophobic surfaces by application of the moving contact line approach. It was demonstrated that the morphology of nanostructures displays a range of structure variations from root-like to a single wire structure with a high anisotropy and aspect ratio (providing diameters of several nanometers and the length limited by the sample surface dimensions). Such nanostructures can be produced exactly on the spot of interest or can be transferred from the surface where they were produced to any other surfaces by the contact printing technique. A model describing the polymer deposition during the moving contact line processes on hydrophobic surfaces has been proposed. The application of this model provides the ground for an explanation of all the obtained experimental data. Utilizing moving contact line approach aligned one-dimensional polycation structures were fabricated and these structures were used as templates for assembling amphiphile molecules. Quasiperiodic aligned and oriented nanostructures of polyelectrolyte molecules formed in moving droplets were utilized for fabrication of electrically conductive one-dimensional nanowires.

The DNA double helix is inherently a nanoscale wire-like object, possessing a 2 nm diameter as well as a remarkable capability for molecular recognition and the interaction with other chemical compounds, thus making it an attractive material for biologically driven assembly of artificial nanostructures. In this work methods for the construction of functional electronic networks from single DNA molecules are presented. For this, (i) the generation of patterns of distinct interconnects between micro-fabricated contact pads are explored by stretching end-specifically thiol-functionalized, single-tethered DNA molecules using hydrodynamic flow as well as an electric field-induced thermal flow. (ii) These networks then serve as a template for a selective in-situ photoinduced nucleation and growth of platinum clusters of 4 nm diameter along the DNA molecules. In the synthesis exclusively platinum ions from an aqueous platinum nitrate solution bonded electrostatically to the backbone of the immobilized DNA can be reduced upon irradiation with UV light, while background metallization is inhibited. Furthermore, the metallization scheme is applied to DNA nanotubes and another photochemical deposition process is used to tune the interparticle gap space in a discontinuous platinum cluster chain to form conducting nanowires. The "process toolbox'' presented in this work offers a versatile alternative for the hierarchical patterning and incorporation of biotemplated nanomaterials into micro-/nanofabrication schemes. / Ein doppelhelikaler DNA-Strang besitzt mit seinem hohen Aspektverhältnis von Natur aus Ähnlichkeit mit einem Kabel. Zusammen mit seinen einzigartigen Selbstassemblierungseigenschaften sowie der Fähigkeit, mit einer Vielzahl von chemischen Stoffen eine Verbindung einzugehen, macht dies ihn zu einem aussichtsreichen Baumaterial für den Aufbau von künstlichen Nanostrukturen. In dieser Arbeit werden deshalb verschiedene Methoden für den Bau von elektronischen Schaltkreisen aus einzelnen DNA-Strängen demonstriert. Dazu wird (i) die Herstellung von Verdrahtungsmustern zwischen lithographisch gefertigten Kontaktstrukturen untersucht. Endständig mit Thiolgruppen funktionalisierte DNA-Moleküle, die an nur einem Ende mit der Oberfläche verknüpft sind, werden mittels Strömung oder eines elektrothermisch induzierten Flusses zwischen Elektroden gespannt. (ii) Diese Netzwerke dienen im Weiteren als Vorlage für ein selektives, lichtinduziertes Wachstum von Platinpartikeln mit Durchmessern von 4 nm lokal entlang der DNA-Moleküle. Dabei werden unter UV-Bestrahlung nur solche Platinionen reduziert, die aus einer Platinnitrat-Lösung elektrostatisch an die immobilisierte DNA angebunden haben. Partikelwachstum in der umgebenden Lösung wird weitgehend verhindert. Darüber hinaus wird dieses Verfahren auch auf DNA-Nanoröhren angewendet und ein weiterer photochemischer Abscheideprozess eingesetzt, um unterbrochene Clusterkettern zusammenzuwachsen, mit dem Ziel, elektrisch leitfähige Nanodrähte zu erhalten. Die vorgestellten Verfahren stellen eine vielseitige Alternative zu herkömmlichen, hierarchischen Fabrikationsschemen der Mikro- und Nanotechnologie dar.

Nanomanufacturing is critical to the future growth of U.S. manufacturing. Yet the process yield of current nanodevices is typically 10% or less. Particularly in nanomaterials growth, there may exist large variability across the sites on a substrate, which could lead to variability in properties. Essential to the reduction of variability is to mathematically describe the spatial variation of nanostructure. This research therefore aims at a method of modeling and estimating nanostructure morphology variation for process yield improvement. This method consists of (1) morphology variation modeling based on Gaussian Markov random field (GMRF) theory, and (2) maximum likelihood estimation (MLE) of morphology variation model based on measurement data. The research challenge lies in the proper definition and estimation of the interactions among neighboring nanostructures. To model morphology variation, nanostructures on all sites are collectively described as a GMRF. The morphology variation model serves for the space-time growth model of nanostructures. The probability structure of the GMRF is specified by a so-called simultaneous autoregressive scheme, which defines the neighborhood systems for any site on a substrate. The neighborhood system characterizes the interactions among adjacent nanostructures by determining neighbors and their influence on a given site in terms of conditional auto-regression. The conditional auto-regression representation uniquely determines the precision matrix of the GMRF. Simulation of nanostructure morphology variation is conducted for various neighborhood structures. Considering the boundary effects, both finite lattice and infinite lattice models are discussed. The simultaneous autoregressive scheme of the GMRF is estimated via the maximum likelihood estimation (MLE) method. The MLE estimation of morphology variation requires the approximation of the determinant of the precision matrix in the GMRF. The absolute term in the double Fourier expansion of a determinant function is used to approximate the coefficients in the precision matrix. Since the conditional MLE estimates of the parameters are affected by coding the date, different coding schemes are considered in the estimation based on numerical simulation and the data collected from SEM images. The results show that the nanostructure morphology variation modeling and estimation method could provide tools for yield improvement in nanomanufacturing.

Recently, developments in novel and high-purity materials allow for the presence of a single, solitary crystalline defect to define the electronic, magnetic, and optical functionality of a device. The discrete nature of the active dopant, whose properties are defined by a quantum mechanical description of its structure, enables radically new quantum investigations and applications in these arenas. Finally,there has been significant development in large-scale device engineering due to mature semiconductor manufacturing techniques. The diverse set of photonic device architectures offering light confinement, guiding, and extraction is a prime example. These three paradigms – solitary dopant photonics and optoelectronics (solotronics), quantum science and technology, and device engineering – merge in the development of novel quantum photonic devices for the next generation of information processing systems. We present in this thesis a series of investigations of optical nanostructures for single optically active spins in single crystal diamond. Chapter 1 introduces the Nitrogen-Vacancy (NV) color center, summarizes its applications, and motivates the need for their integration into photonic structures. Chapter 2 describes two prototype nanobeam photonic crystal cavities for generating strong light-matter interactions with NV centers. The first device consists of a silicon nitride photonic crystal nanobeam cavity with high quality factor \(Q \sim 10^5\) and small mode volume \(V \sim 0.5*(\lambda/n)^3\). The second device consists of a monolithic diamond nanobeam cavity fabricated with the focused ion beam (FIB) directly in a single crystal diamond sample. Chapter 3 presents a high-efficiency source of single photons consisting of a single NV center in a photonic diamond nanowire. Early FIB prototypes are described, as is the first successful realization of the device achieved via reactive ion etching nanowires in a single crystal diamond containing NV centers, and finally a variation of this approach based on incorporation of NV centers in pure diamond via ion implantation. In chapter 4 we consider the optimal design of photonic devices offering both collection efficiency and cavity-enhancements and extend the model of the NV center to include photonic effects. In chapter 5 we briefly introduce a novel optically active spin discovered in a diamond nanowire. Finally, in chapter 6 we conclude with several proposals to extend this research program. / Engineering and Applied Sciences

Central to the implementation of colloidal nanomaterials in commercial applications is the development of high throughput synthesis strategies for technologically relevant materials. Solution based synthesis approaches provide the controllability, high throughput, and scalability needed to meet commercial demand. A flow through supercritical fluid reactor was used to synthesize silicon nanowires in high yield with production rates of ~45 mg/hr. The high temperature and high pressure of the supercritical medium facilitated the decomposition of monophenylsilane and seeded growth of silicon nanowires by gold seeds. Crystalline nanowires with diameters of ~25 nm and lengths greater than 20 [micrometers] were routinely synthesized. Accumulation of nanowires in the reactor resulted in deposition of a conformal amorphous shell on the crystalline surface of the wire. X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and energy dispersive X-ray spectroscopy were used to determine the shell composition. The shell was identified as polyphenylsilane formed by polymerization of the silicon precursor monophenylsilane. A post synthesis etch was developed to remove the shell while still maintaining the integrity of the crystalline silicon nanowire core. Subsequent surface passivation was achieved through thermal hydrosilylation with a terminal alkene. The development colloidal nanomaterials into commercial applications also requires simple and robust bottom-up assembly strategies to facilitate device fabrication. A Langmuir-Blodgett trough was used to assemble continuous monolayers of hexagonally ordered spherical nanocrystals over areas greater than 1 cm². Patterned monolayers and multilayers of FePt nanocrystals were printed onto substrates using pre-patterned polydimethylsiloxane (PDMS) stamps and a modified Langmuir Schaefer transfer technique. Patterned features, including micrometer-size circles, lines, and squares, could be printed using this approach. The magnetic properties of the printed nanocrystal films were also measured using magnetic force microscopy (MFM). Room temperature MFM could detect a remanent (permanent) magnetization from multilayers (>3 nanocrystals thick) films of chemically-ordered L1₀ FePt nanocrystals. Grazing incidence small angle X-ray scattering was used to quantitatively characterize the grain size, crystal structure, lattice disorder, and edge-to-edge spacing of the nanocrystal films prepared on the Langmuir-Blodgett trough both on the air-water interface and after transfer. / text

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The electrical properties of nanowire-based n-InSb-n-InAs heterojunctions grown by chemical beam epitaxy were investigated both theoretically and experimentally. This heterostructure presented a type-III band alignment with the band bendings at 0.12 eV for InAs side and 0.16 − 0.21 eV in InSb. Analysis of the temperature dependent current voltage characteristics showed that the current through the heterojunction is caused mostly by generation-recombination processes in the InSb and at the heterointerface. Due to the partially overlapping valence band of InSb and the conduction band of InAs, the second process was fast and activationless. Theoretical analysis showed that, depending on the heterojunction parameters, the flux of non-equilibrium minority carriers may have a different direction, explaining the experimentally observed non-monotonic coordinate dependence of the electron beam induced current at the vicinity of heterointerface.

The electrical properties of nanowire-based n-InSb-n-InAs heterojunctions grown by chemical beam epitaxy were investigated both theoretically and experimentally. This heterostructure presented a type-III band alignment with the band bendings at 0.12 eV for InAs side and 0.16 − 0.21 eV in InSb. Analysis of the temperature dependent current voltage characteristics showed that the current through the heterojunction is caused mostly by generation-recombination processes in the InSb and at the heterointerface. Due to the partially overlapping valence band of InSb and the conduction band of InAs, the second process was fast and activationless. Theoretical analysis showed that, depending on the heterojunction parameters, the flux of non-equilibrium minority carriers may have a different direction, explaining the experimentally observed non-monotonic coordinate dependence of the electron beam induced current at the vicinity of heterointerface.