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Atomic vapors condensed onto solid surfaces form a remarkable category of condensed matter materials, the so-called thin films, with a myriad of compositions, morphological structures, and properties. The dynamic process of atomic condensation exhibits self-assembled pattern formation, producing morphologies with atomic-scale three-dimensional structures of seemingly limitless variety. This study attempts to shed new light on the dynamical growth processes of thin film deposition by analyzing in detail a previously unreported specific distinct emergent structure, a crystalline triangular-shaped spike that grows within copper and silver thin films. I explored the deposition parameters that lead to the growth of these unique structures, referred to as ``nanospikes'', fabricating approximately 55 thin films and used scanning electron microscopy and x-ray diffraction analysis. The variation of parameters include: vapor incidence angle, film thickness, substrate temperature, deposition rate, deposition material, substrate, and source-to-substrate distance. Microscopy analysis reveals that the silver and copper films deposited at glancing vapor incidence angles, 80 degrees and greater, have a high degree of branching interconnectivity between adjacent inclined nanorods. Diffraction analysis reveals that the vapor incidence angle influences the sub-populations of crystallites in the films, producing two different [110] crystal texture orientations. I hypothesize that the growth of nanospikes from nanorods is initiated by the stochastic arrival of vapor atoms and photons emitted from the deposition source at small diameter nanorods, and then driven by localized heating from vapor condensation and photon absorption. Restricted heat flow due to nanoscale thermal conduction maintains an elevated local temperature at the nanorod, enhancing adatom diffusion and enabling fast epitaxial crystal growth, leading to the formation and growth of nanospikes. Electron microscopy and x-ray diffraction analysis, and comparisons to related scientific literature, support this hypothesis. I also designed a highly modular ultrahigh vacuum deposition chamber, capable of concurrently mounting several different pieces of deposition equipment, that allows for a high degree of control of the growth dynamics of deposited thin films. I used the newly designed chamber to fabricate tailor-made nanostructured tantalum films for use in ultracapacitors, for the Cabot Corporation. / Thesis (Ph.D, Physics, Engineering Physics and Astronomy) -- Queen's University, 2011-01-17 15:22:47.533

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Although molybdenum blue solutions have been known for more than twocenturies, an understanding of their chemical nature is only beginning to emerge.This dissertation aimed at elucidating the structural nature of the polydisperse,nanoscopic components in the solution phases and the solid states of partiallyreduced polyoxomolybdate (Mo-POM). The study offered at least fourcontributions to the area: (1) a rational protocol for the molecular recognition ofMo-POM with de novo organic hosts. (2) demonstration of kinetic precipitation ofa dynamic mixture of polyoxomolybdates and application of the technique to thestudy of the dynamic mixture by TEM (3) characterization of the Mo-POMnanostructures by an unusual combination of complementary analyticaltechniques. (4) a general approach for the synthesis of crown-ethers-containingtripodal molecules.The molecular recognition of Mo-POM with designer tripodal hexaminetris-crown ethers opened a window to the solution phase structures of Mo-POMnanoscopic components. Studies with a series of structurally analogous hostsprobed the relationship between the structure of the molecular host and theformation of nanostructures.An unusual combination of complementary analytical protocols: flow fieldflowfractionation, electron microscopy (transmission and scanning), andinductively coupled plasma – emission spectroscopy, was used to monitor thesolution-phase evolution of Mo-POM nanostructures. The crystallization – drivenformation of keplerate Mo-POM and solution-phase evolution of structurallyrelated nanoscopic species were apparent in the self-assembling process ofpartially reduced Mo-POM.

Photonic cavities are able to confine light to a volume of the order of wavelength of light and this ability can be described in terms of the cavity’s quality factor, which in turn, is proportional to the confinement time in units of optical period. This property of the photonic cavities have been found to be very useful in cavity quantum electrodynamics, for e.g., controlling emission from strongly coupled single photon sources like quantum dots. The smallest possible mode volume attainable by a dielectric cavity, however, poses a limit to the degree of coupling and therefore to the Purcell effect. As metal nanoparticles with plasmonic properties can have mode volumes far below the diffraction limit of light, these can be used to achieve stronger coupling, but the lossy nature of the metals can result in extremely poor quality factors. Hence a hybrid approach, where a high-quality dielectric cavity is combined with a low-quality metal nanoparticle, is being actively pursued. Such structures have been shown to have the potential to preserve the best of both worlds. This thesis describes the design, fabrication and characterization of hybrid plasmonic – photonic nanobeam cavities. Experimentally, we were able to achieve a quality factor of 1200 with the hybrid approach, which suggests that the results are promising for future single photon emission studies. It was found that modeling the behaviour (resonant frequencies, quality factors) of these hybrid cavities with conventional computation methods like FDTD can be tedious, for e.g., a comprehensive study of the electromagnetic fields inside a hybrid photonic nanobeam cavity has been found to take up to 48 hours with FDTD. Hence, we also present an alternate method of analysis using perturbation theory, showing good agreement with FDTD. / Graduate

High energy neutron and charged particle radiation cause microstructural and mechanical degradation in structural metals and alloys, such as phase segregation, void swelling, embrittlement and creep. Radiation induced damages typically limit nuclear materials to a lifetime of about 40 years. Next generation nuclear reactors require materials that can sustain over 60 - 80 years. Therefore it is of great significance to explore new materials with better radiation resistance, to design metals with favorable microstructures and to investigate their response to radiation. The goals of this thesis are to study the radiation responses of several nanostructured metallic thin film systems, including Ag/Ni multilayers, nanotwinned Ag and nanocrystalline Fe. Such systems obtain high volume fraction of boundaries, which are considered sinks to radiation induced defects. From the viewpoint of nanomechanics, it is of interest to investigate the plastic deformation mechanisms of nanostructured films, which typically show strong size dependence. By controlling the feature size (layer thickness, twin spacing and grain size), it is applicable to picture a deformation mechanism map which also provides prerequisite information for subsequent radiation hardening study. And from the viewpoint of radiation effects, it is of interest to explore the fundamentals of radiation response, to examine the microstructural and mechanical variations of irradiated nanometals and to enrich the design database. More importantly, with the assistance of in situ techniques, it is appealing to examine the defect generation, evolution, annihilation, absorption and interaction with internal interfaces (layer interfaces, twin boundaries and grain boundaries). Moreover, well-designed nanostructures can also verify the speculation that radiation induced defect density and hardening show clear size dependence. The focus of this thesis lies in the radiation response of Ag/Ni multilayers and nanotwinned Ag subjected to charged particles. The radiation effects in irradiated nanograined Fe are also investigated for comparison. Radiation responses in these nanostructured metallic films suggest that immiscible incoherent Ag/Ni multilayers are more resistant to radiation in comparison to their monolithic counterparts. Their mechanical properties and radiation response show strong layer thickness dependence in terms of radiation hardening and defect density. Coherent twin boundaries can interact with stacking fault tetrahedral and remove them effectively. Twin boundaries can actively absorb radiation induced defects and defect clusters resulting in boundary migration. Size dependence is also found in nanograins where fewer defects exhibit in films with smaller grains.