Pulsed lasers are studied as new tools to realize competitive nanomanufacturing. The capabilities of pulsed lasers as promising tools for research, design, manufacturing, and control rely on the flexibility due to the great variety of operation parameters, and the inherent precision in aspects of time, spatial resolution, and energy input. As new tools, the fundamental understanding and technological capabilities of pulsed laser-induced chemical synthesis were explored in this dissertation research. In order to study the capabilities of pulsed laser in controlled synthesis, a thermal model was developed to predict the local temperature change due to the very short period of irradiation by a pulsed laser. And combining with the classical Gibbs free energy theories, a set of guidelines were developed for precision control for pulsed laser-induced chemical synthesis. Zinc oxide crystals were studied as an example case, showing the relationship between the wide range variables of pulsed laser including repetition rate, energy area density, power density, irradiation duration, etc. and the material structures of deposited crystals in aspects of crystal density, size, shape, crystalline properties, surface morphologies, growth rate, etc. Mechanisms from thermodynamic and kinetic aspects were explored. Pulsed laser-induced different heating conditions were found to separate two crystallization processes with different energy barriers, one dominated by a burst of nucleation and the other dominated by crystal growth through particle aggregation. For the study of the fundamental mechanisms in crystallization, pulsed laser initiated and controlled the crystallization in its early stage, and the crystal evolution were observed and analyzed by transmission electron microscopy (TEM). Crystal growth from intermediate monomers was first studied by an electron beam under the condition without precursor solution environment, providing crucial process information of crystal evolution, indicating multistage processes by continuous mass and phase transfer among intermediate monomers. This dissertation shows the capabilities of pulsed laser in realizing precision control for the targeted synthesis in nanomanufacturing, providing unique insight to crystallization mechanisms, and extending prospects to scientific research of other energy beam induced processes.

<p>  </p> <p>This masters thesis presents a literature review of widely used ink-based manufacturing techniques, ink-based materials used in energy harvesting. their preparation and applications in human-integrated energy harvesting devices. In addition, the challenges, and opportunities in this area of study is discussed. Lastly, the experimental methodology and results of a stencil printed PVA-gelatin composite ink based flexible triboelectric nanogenerator used for human-integrated energy harvesting is summarized.</p>

Development of nanoscience and nanotechnology requires rapid and robust nanomanufacturing processes to produce nanoscale materials, structures and devices. The dissertation aims to contribute to two major challenging and attractive topics in nanomanufacturing. Firstly, this research develops fabrication techniques for three dimensional (3D) structures and integrates them into functional devices and systems. Secondly, a novel process is proposed and studied for rapid and efficient manipulation of nanomaterials using a directed self-assembly process. The study begins with the development of nanoimprint lithography for nanopatterning and fabrication of 3D multilayer polymeric structures in the micro- and nano-scale, by optimizing the layer-transfer and transfer-bonding techniques. These techniques allow the integration of microfluidic and photonic systems in a single chip for achieving ultracompact lab-on-a-chip concept. To exemplify the integration capability, a monolithic fluorescence detection system is proposed and the approaches to design and fabricate the components, such as a tunable optical filter and optical antennas are addressed. The nanoimprint lithography can also be employed to prepare nanopatterned polymer structures as a template to guide the self-assembly process of nanomaterials, such as single-walled carbon nanotubes (SWNTs). By introducing the surface functionalization, electric field and ultrasonic agitation into the process, we develop a rapid and robust approach for effective placement and alignment of SWNTs. These nanomanufacturing processes are successfully developed and will provide a pathway to the full realization of the lab-on-a-chip concept and significantly contribute to the applications of nanomaterials.

Additive manufacturing using 2 photon polymerization is of great interest as it can create nanostructures with feature sizes much below the diffraction limit. It can be called as true 3D printing as it can fabricate in 3 dimensions by moving the laser spot in any 3D pattern inside the resist. This unique property is attributed to the non-linearity of two photon absorption which makes the polymerization happen only at the focal spot of the laser beam. This method has a wide range of applications such as optics/photonics, metamaterials, metasurfaces, micromachines, microfluidics, tissue engineering and drug delivery.<br>This work focuses on utilizing 2 photon fabrication for creating a metasurface by printing diabolo antenna arrays on a glass substrate and subsequently metallizing it by coating with gold. A femtosecond laser is used along with a galvo-mirror to scan the geometry inside the photoresist to create the antenna. The structure is simulated using ANSYS HFSS to study its properties and optimize the parameters. The calculations show a reflectance dip and zero reflectance for the resonance condition of 4.04 μm. An array of antennas is fabricated using the optimized properties and coated with gold using e-beam evaporation. This array is studied using a fourier transform infrared spectrometer and polarization dependent reflectance dip to 40% is observed at 6.6 μm. The difference might be due to the small errors in fabrication. This method of 3D printing of antenna arrays and metallization by a single step of e-beam evaporation is hence proved as a viable method for creating optical metasurfaces. Areas of future research for perfecting this method include incorporating an autofocusing system, printing more complicated geometries for antennas, and achieving higher resolution using techniques like stimulated emission depletion.

The thesis systematically investigates the laser interference nanomanufacturing technology taking into account its advantages and abilities to realise various potential applications. The latest progresses have addressed the major issues hampering the cross-scale developments of structural applications, such as cost-ineffective fabrication, limited area, low efficiency and challenging integration. The studies carried out on high-resolution and large-area laser interference nanomanufacturing technology will complement the exploration of modern optical devices and extraordinary functional applications. With respect to classical interference theory and relevant references, there is still a lack of studies providing insight into the effects of polarisation on the multi-beam interference while it is found that the polarisation vector plays a key role in the formation, period and contrast of interfering patterns. Herein, the theory of multi-beam interference is developed through the integration of the polarisation vector and electric field vector. It is worth pointing out that based on the detailed analysis of the four-beam interference with the special polarisation modes, it is demonstrated that the modulation phenomenon in four-beam laser interference is the result of the misalignment of incident angles or unequal incident angles only in the case of the TE-TE-TM-TM mode. In the experiments, a straightforward method of generating various well-defined structures on material surfaces is proposed using the nanosecond laser interference system. The experimental results of two-, three- and four-beam interference show a good correspondence to the theoretical analyses and simulations. Artificial bio-structures are fabricated using the four-beam interference method with the TE-TE-TE-TE polarisation mode and the fabricated microcone structures exhibit excellent properties with both a high contact angle (CA=156.3°) and low omnidirectional reflectance (5.9-15.4%). In order to fabricate high-resolution structures, the 266nm nanosecond laser interference system is employed to treat the organic and metal-film materials. Nanograting structures with feature sizes of sub-100nm width and 2nm height are fabricated on the organic material surface. An attempt is successfully conduced to produce the nanoelectrode arrays by using laser interference lithography and chemical deposition. Finally, the advantages of the developed laser interference technology and contributions of the research are summarised, and recommendations of future work are given.

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The ability to pattern in the nanoscale to drill holes, to draw lines, to make circles, or more complicated shapes that span a few atoms in width is the main driver behind current efforts in the rapidly growing area of nanomanufacturing. In applications ranging from the microprocessor industry to biomedical science, there is a constant need to develop new tools and processes that enable the shrinking of devices. For this and more applications, nanomanufacturing using electron beams offers a window of opportunity as a top-down approach since electrons, unlike light, have a wavelength that is in the order of the atomic distance. Though the technology based on electron beams has been available for more than twenty years, new concepts are constantly being explored and developed based on fundamental approaches. As such, a tool that utilizes electron field-emission from carbon nanotubes was proposed to accomplish such feats. A full numerical analysis of electron field-emission from carbon nanotubes for nanomachining applications is presented. The different aspects that govern the process of electron field-emission from carbon nanotubes using the finite element method are analyzed. Extensive modeling is carried here to determine what the effect of different carbon nanotube geometries have on their emission profiles, what energy transport processes they are subject to, and establish what the potential experimental parameters are for nanomachining. This dissertation builds on previous efforts based on Monte Carlo simulations to determine electron deposition profiles inside metals, but takes them to next level by considering realistic emission scenarios. A hybrid numerical approach is used that combines the two-temperature model with Molecular Dynamics to study phase change and material removal in depth. The use of this method, allows the determination of the relationship between the amount of energy required to remove a given number of atoms from a metallic workpiece and the number of carbon nanotubes and their required settings in order to achieve nanomachining. Finally, the grounds for future work in this area are provided, including the need for novel electron focusing systems, as well as the extension of the hybrid numerical approach to study different materials.

Understanding and manipulating nanosized particles is crucial for the advancement of nanotechnology research. Dependent light scattering of noble metals can be used to achieve new material responses that can be used in different applications. Dependent light scattering of nanoparticles allows the understanding of orientation and location of closely positioned particles. Besides, dependently scattering metallic particles create significantly enhanced near fields and high absorption rates when excited at their plasmon resonance. It is used for spectrally selective heating and melting of nanosized particles as a nanomanufacturing method. With numerical methods dependent scattering properties of particles can be obtained. In this study, the dependent optical absorption efficiencies of metallic nanoparticles are obtained with the newly developed Integrated Poynting Vector Approach (IPVA). This is used in conjunction with a numerical light scattering solution tool DDSCAT. Results indicate that IPVA and DDSCAT together can be used for the estimation of scattering and absorption of nanoparticles affected by the near field of other particles in their close vicinity. The method is suggested to be suitable for the understanding of physical mechanisms behind dependent scattering prior to experiments that require lots of effort and resources.

Polyvinylidene difluoride (PVDF) is a functional polymeric material that can be used for a wide variety of applications. There are many new future applications that were recently suggested for electrospun PVDF fibers. Electrospinning is a process capable of producing nano to micro sized PVDF fibers in a web. It is important to control the structure of the web during electrospinning because by controlling the structure of the web it is possible for the PVDF fiber web to have increased performance in comparison to other common forms of PVDF. While past scientific literature focused on applications of PVDF fibers, little was known on how to control structure of PVDF fiber webs during production. Even though defects can alter the structure and performance of the web only a few studies reported defect occurrence and how to reduce the occurrence of defects in fiber webs. This research investigated the defect free production space of electrospun PVDF and provided streamlined guidelines for manufacturers to use for electrospinning PVDF webs. Many studies looked at influencing fiber diameter and beading with one factor at a time experimentation; this work was foundational and was able to identify many important electrospinning parameters. But this methodology neglected the possibility of parameter interactions and often did not look at the effects of parameters on the occurrence of defects and the structure of those defects. Therefore a systematic understanding that included all of the important electrospinning parameters in relation to fiber and defect structure was needed to present a clear picture of the possibilities for controlling the structure of electrospun PVDF webs. This research explored ways to control the structure of PVDF fiber webs. The production space and control of web structure was explored by using a regression analysis to identify important parameters and interactions. Then the regression analysis was used to determine the effects of the important parameters that influenced the web structure. This research showed that the web structure can be controlled using solution parameters and processing parameters and monitored by system parameters. In addition, this study showed that by controlling the web structure it was possible to influence the porosity and piezoelectric properties of PVDF fiber webs. In its entirety, this research presents a systematic approach to producing PVDF fibers for tailored web performance.

Electrospray is an atomization method subject to intense study recently due to its monodispersity and the wide size range of droplets it can produce, from nanometers to hundreds of micrometers. This thesis focuses on the numerical and theoretical modeling of the interaction of charged droplets from the single and multiplexed electrospray. We studied two typical scenarios: large area film depositions using multiplexed electrospray and fine pattern printings assisted by linear electrostatic quadrupole focusing. Due to the high computation power requirement in the unsteady n-body problem, graphical processing unit (GPU) which delivers 10 Tera flops in computation power is used to dramatically speed up the numerical simulation both efficiently and with low cost. For large area film deposition, both the spray profile and deposition number density are studied for different arrangements of electrospray and electrodes. Multiplexed electrospray with hexagonal nozzle configuration can not give us uniform deposition though it has the highest packing density. Uniform film deposition with variation < 5% in thickness was observed with the linear nozzle configuration combined with relative motion between ES source and deposition substrate. For fine pattern printing, linear quadrupole is used to focus the droplets in the radial direction while maintaining a constant driving field at the axial direction. Simulation shows that the linear quadrupole can focus the droplets to a resolution of a few nanometers quickly when the interdroplet separation is larger than a certain value. Resolution began to deteriorate drastically when the inter-droplet separation is smaller than that value. This study will shed light on using electrospray as a scalable nanomanufacturing approach.