Driven by the emerging interest in the design and realization of structures with co-existing micro- and nanoscale features, various nanofabrication approaches are being developed. We show that the selective, conformal growth of a multilayer structure is a promising route for the controlled realization of various structures with size-hierarchy, including both surface (i.e., the structures of which functionalities are characterized by the interaction between their surface, and external systems, such as self-cleaning, superhydrophic substrates with dual-scale topography), and volumetric (i.e. composite materials of which functionalities rely on the intrinsic properties of nanostructures distributed throughout their volume, such as giantmagnetoresistance sensors) structures. This is realized based on a sequential multilayer electrodeposition guided by an insulating substrate with predesigned topography, referred to as template-assisted multilayer electrodeposition process. Various multiscale, multidimensional surface and volumetric hierarchical structures are demonstrated of which size scale of the nanostructures are defined by the individual layer deposition parameters, while their position and overall geometry are defined by that of the template. These structures include (1) large area (> 1 cm^2), planar, or non-planar surfaces comprised of anisotropic, nanoscale surface relief structures of wide-ranging size scale (10 nm-1 micron); and (2) thick (10-100 micron), volumetric composite material in which individual metallic layers of micron, or submicron scale thicknesses are electrically insulated from the adjacent layers by interlamination insulating layers of similar thicknesses. The utility of the fabricated structures is evaluated in a few potential application domains, i.e., nanolithography, self-cleaning, and high frequency magnetic devices.

The success of many emerging biotechnologies depends upon the ability to tune cell function to mimic conditions found in vivo. Cells exhibit complex interactions with their surrounding environment known and the extracellular matrix (ECM). These interactions control many cell functions such as proliferation, differentiation and cell death. ECM components span the meso-, micro- and nano-length scales. Successful biotechnologies therefore must also exhibit patterning over these length scales. The objective of this study is to fabricate and analyze cell response to micro and nanopatterned polymer substrates. Experiments examined cell alignment and proliferation to various substrates. The substrates used featured micropatterned grooves and holes, micropatterned carbon nanotubes, and combinations of microgrooves and nanogrooves. Results showed significant interactions between cell alignment and the patterned topography for all substrate types, while cell proliferation showed no significant dependence on these topographic parameters.

Towards the creation of the next generation of biomedical implants that effectively integrate in tissues, understanding cell behaviour at the material-host interface to control and optimize the biological outcome is a crucial endeavour. It is now well known that the nanoscale surface properties of biomaterials play a significant role in directing the activity of adherent cells at the implant-host tissue interface. A variety of cellular functions, ranging from adhesion and proliferation to differentiation along specific lineages, are guided by the nanoscale topographical and physicochemical features of the substrate. This evidence reaffirms the role of surface features on eliciting an enhanced response of cells towards improved biological outcomes (e.g., bone integration) of implanted biomaterials. In this context, Titanium (Ti) and its alloys are popular biomaterials widely used in orthopedic, dental, and cardiovascular applications. In particular, in the field of osseointegrated devices, chemical treatments of titanium, specifically oxidative nanopatterning (i.e., a simple yet effective treatment with a H₂SO₄/H₂O₂ solution), have shown to be a promising strategy for guiding and controlling the fate of relevant cells (e.g., osteoblasts, stem cells), thereby achieving the ability to direct the biological response towards the desired outcome. In this context, the sponge-like nanoporous surface resulting from oxidative nanopatterning of titanium allows direct surface cueing to bone cells. It also has the capacity to selectively regulate cell behaviour, modulate the expression of crucial determinants of cell activity, and offers the potential to harness the power of stem cells. However, the mechanisms that control how cells sense and respond to these nanometric cues are still elusive. A novel strategy to elucidate them takes inspiration from in-vivo protocols, where "knock-out" animal models are used to determine the role of a specific gene. Based on this, I propose an original approach aimed at investigating cell response under conditions known to affect specific cellular processes, thereby determining whether these activities can be rescued by direct cueing by the substrate, ultimately elucidating their implication in responding to a given nanostructured substrate. In particular, hyperglycemic culturing conditions often used to mimic diabetes in-vitro are known to exert detrimental effects on the proliferation and differentiation of osteoblasts, and thereby could be an excellent opportunity to test whether the nanometric surface features resulting from oxidative nanopatterning of titanium also possess the ability to compensate to the cell-level changes caused by higher levels of glucose. This would ultimately demonstrate a direct effect of the substrate on these events and help us understand the mechanisms involved in cell-biomaterial interactions. To address this challenge, I propose to investigate the response of human MG-63 osteoblastic cells to nanoporous titanium under hyperglycemic conditions. The goal is, therefore, to understand whether direct nanotopographical cueing at the nanoscale can rescue MG-63 cells from the effects of hyperglycemia, thereby casting new light on the mechanisms underlying the interactions between this widely used cell line and nanoporous titanium. In parallel, results from my work aim at providing new fundamental evidence to interpret results from that body of literature that uses high glucose content as a way to mimic the osseointegration of biomaterials in diabetic conditions.

A high-speed, large-area technique capable of nanopatterning flexible substrates is highly desirable in several applications such as; 1) thin film photovoltaics (TFPV's), 2) flexible electronics, 3) optoelectronics, 4) energy storage devices and 5) biological applications. Flexible substrates are attractive as they can be lower in cost than traditional substrates, and provide the ability to perform continuous processing both of which are valuable for cost sensitive applications such as TFPVs. Also, flexible substrates can conform to non-planar surfaces and therefore provide versatility in applications such as wearable electronics and biomedical devices. In this thesis, a patterning approach known as Jet and Flash Imprint Lithography (J-FIL) is explored for flexible substrates. J-FIL uses inkjets to deposit low-viscosity UV curable polymer materials (resists) that are molded by a template at room temperature and low pressures prior to UV cross-linking. There are inherent advantages to the J-FIL process that lends itself to patterning flexible substrates. The room temperature and low pressure process makes it more compatible with flexible substrates which tend to become dimensionally unstable at elevated temperatures and pressure. The extension of J-FIL to flexible substrates involves the following key challenges: (i) Understanding the level of precision required in roll-to-roll machine systems to ensure that these systems can facilitate imprint and separation of nano-scale features; (ii) The substrate surface should be controlled to initiate and maintain proper interface with the template and avoid formation of bubbles; (iii) The tension in the film should be controlled to ensure that the discrete resist drops are coerced to form a uniform contiguous residual film underneath the patterns; (iv) The fluid filling time - that is representative of the process throughput - should be low; and (v) After UV curing and separation, the nanoscale patterns should not be deformed or damaged. The above challenges were addressed by developing a roll-to-roll test bed to imprint flexible polycarbonate films using the J-FIL process. The test bed has the capability of controllably varying a number of web tension parameters as well as process variables in order to calibrate machine precision and establish control schemes for a robust process. Process metrics such as RLT uniformity, target RLT accuracy, feature filling and feature distortion were measured and quantified. A design of experiments was performed on the test bed for the purposes tuning the process variables as well as developing a model of process performance, with respect to critical process parameters. A two-level design, with three input variables, is utilized in this experimental process. The process yielded blank imprints with mean thickness of 70.5 nm, and a standard deviation of 3.9 nm. The sensitivity of the mean thickness and uniformity to process variables were quantified. The best performing set of input parameters were then used during patterned imprints, to determine if any pattern filling issues or pattern deformation would take place. The patterned imprints, made up of an array of hexagonal pillars (125nm tall, by 240 nm wide, by 450 nm pitch) showed no sign of fluid filling voids, or deformation due to separation. Given this result, the feasibility of implementing J-FIL on a roll-to-roll prototype system was established. A proposed next generation flexible substrate J-FIL tool is presented, along with the expected challenges associated with metrology and dynamic noise. Future work entails the design and qualification of a full scale roll-based imprint tool, capable of meeting throughput metrics established for industrial applications. / text

<p>Today, the dominating way of patterning nanosystems is by irradiation-based lithography (e-beam, DUV, EUV, and ions). Compared to the other irradiations, ion tracks created by swift heavy ions in matter give the highest contrast, and its inelastic scattering facilitate minute widening and high aspect ratios (up to several thousands). Combining this with high resolution masks it may have potential as lithography technology for nanotechnology. Even if this ‘ion track lithography’ would not give a higher resolution than the others, it still can pattern otherwise irradiation insensitive materials, and enabling direct lithographic patterning of relevant material properties without further processing. In this thesis ion tracks in thin films of polyimide, amorphous SiO₂ and crystalline TiO₂ were made. Nanopores were used as templates for electrodeposition of nanowires.</p><p>In lithography patterns are defined by masks. To write a nanopattern onto masks e-beam lithography is used. It is time-consuming since the pattern is written serially, point by point. An alternative approach is to use self-assembled patterns. In these first demonstrations of ion track lithography for micro and nanopatterning, self-assembly masks of silica microspheres and porous alumina membranes (PAM) have been used. </p><p>For pattern transfer, different heavy ions were used with energies of several MeV at different fluences. The patterns were transferred to SiO₂ and TiO₂. From an ordered PAM with pores of 70 nm in diameter and 100 nm inter-pore distances, the transferred, ordered patterns had 355 nm deep pores of 77 nm diameter for SiO₂and 70 nm in diameter and 1,100 nm deep for TiO₂. The TiO₂ substrate was also irradiated through ordered silica microspheres, yielding different patterns depending on the configuration of the silica ball layers. </p><p>Finally, swift heavy ion irradiation with high fluence (above 10¹⁵/cm²) was assisting carbon nanopillars deposition in a PAM used as template. </p>

Today, the dominating way of patterning nanosystems is by irradiation-based lithography (e-beam, DUV, EUV, and ions). Compared to the other irradiations, ion tracks created by swift heavy ions in matter give the highest contrast, and its inelastic scattering facilitate minute widening and high aspect ratios (up to several thousands). Combining this with high resolution masks it may have potential as lithography technology for nanotechnology. Even if this ‘ion track lithography’ would not give a higher resolution than the others, it still can pattern otherwise irradiation insensitive materials, and enabling direct lithographic patterning of relevant material properties without further processing. In this thesis ion tracks in thin films of polyimide, amorphous SiO2 and crystalline TiO2 were made. Nanopores were used as templates for electrodeposition of nanowires. In lithography patterns are defined by masks. To write a nanopattern onto masks e-beam lithography is used. It is time-consuming since the pattern is written serially, point by point. An alternative approach is to use self-assembled patterns. In these first demonstrations of ion track lithography for micro and nanopatterning, self-assembly masks of silica microspheres and porous alumina membranes (PAM) have been used. For pattern transfer, different heavy ions were used with energies of several MeV at different fluences. The patterns were transferred to SiO2 and TiO2. From an ordered PAM with pores of 70 nm in diameter and 100 nm inter-pore distances, the transferred, ordered patterns had 355 nm deep pores of 77 nm diameter for SiO2 and 70 nm in diameter and 1,100 nm deep for TiO2. The TiO2 substrate was also irradiated through ordered silica microspheres, yielding different patterns depending on the configuration of the silica ball layers. Finally, swift heavy ion irradiation with high fluence (above 1015/cm2) was assisting carbon nanopillars deposition in a PAM used as template.

Bacteria in nature predominantly grow as biofilms on living and non-living surfaces. The development of biofilms on non-living surfaces is significantly affected by the surface micro/nano topography. The main goal of this dissertation is to study the interaction between microorganisms and nanopatterned surfaces. In order to engineer the surface with well-defined and repeatable nanoscale structures, a new, versatile and scalable nanofabrication method, termed Spun-Wrapped Aligned Nanofiber lithography (SWAN lithography) was developed. This technique enables high throughput fabrication of micro/nano-scale structures on planar and highly non-planar 3D objects with lateral feature size ranging from sub-50 nm to a few microns, which is difficult to achieve by any other method at present. This nanolithography technique was then utilized to fabricate nanostructured electrode surfaces to investigate the role of surface nanostructure size (i.e. 115 nm and 300 nm high) in current production of microbial fuel cells (MFCs). Through comparing the S. oneidensis attachment density and current density (normalized by surface area), we demonstrated the effect of the surface feature size which is independent of the effect on the surface area. In order to better understand the mechanism of microorganism adhesion on nanostructured surfaces, we developed a biophysical model that calculates the total energy of adhered cells as a function of nanostructure size and spacing. Using this model, we predict the attachment density trend for Candida albicans on nanofiber-textured surfaces. The model can be applied at the population level to design surface nanostructures that reduce cell attachment on medical catheters. The biophysical model was also utilized to study the motion of a single Candida albicans yeast cell and to identify the optimal attachment location on nanofiber coated surfaces, thus leading to a better understanding of the cell-substrate interaction upon attachment. / Ph. D. / Formation of surface associated multicellular communities of microorganisms known as biofilms is of concern in medical settings as well as in industries such as oil refineries and marine engineering. It has been shown that micro/nanoscale surface features can highly regulate the process of biofilm formation and the attached cell activities. In this dissertation, we study the interaction between surface nanoscale structures and bacterial adhesion by experiments and biophysical modelling. We develop the Spun-Wrapped Aligned Nanofiber (SWAN) lithography, a versatile, scalable, and high throughput technique for masterless nanopatterning of hard materials. Using this technique, we demonstrate high fidelity whole surface single step nanopatterning of bulk and thin film surfaces of regularly and irregularly shaped 3D objects. SWAN lithography is used to texturize the electrode surface of microbial fuel cells (MFCs), which are envisioned as an alternative sustainable energy source. Compared to the non-patterned electrodes, the electrodes with 115 nm surface patterns facilitate larger biofilm coverage and 40% higher current production. We also develop a biophysical model to optimally texturize the surface of central venous and uretic medical catheters to prevent biofilm formation by fungal pathogen, Candida albicans. We show that the surface structures that result the highest cell total energy retained the least C. albicans. Furthermore, the adhesion behaviour of a single yeast cell is also experimentally studied in conjunction with the developed model.

Thèse numérisée par la Division de la gestion de documents et des archives de l'Université de Montréal.

Thèse numérisée par la Division de la gestion de documents et des archives de l'Université de Montréal

The bombardment of surfaces by ions can lead to the spontaneous formation of nano-structures. Depending on the irradiation conditions, smoothening or roughening mechanisms can be the leading order in pattern formation which can result in the creation of dots, ripples or ultra-smoothening effects. Because ion bombardment is already ubiquitous in industrial settings, and is relatively inexpensive compared to other surface processing techniques, self-organized patterning by ion bombardment could enable a simple, economical means of inducing well-defined nanoscale structures in a variety of settings. Understanding the fundamental behavior of surfaces during ion bombardment is therefore a vital goal; however, a complete understanding of physical processes governing surface pattern formation has not been reached yet. In order to address this issue, my thesis research has utilized three primary approaches. First, I have done real-time non-coherent X-ray scattering experiments at Cornell High Energy Synchrotron Source (CHESS) for studying kinetics of structure formation of Silicon undergoing Ar⁺ bombardment over a range of wavenumbers 4-5 times larger than has previously been obtained. From our data, we were able to extract values of the angle-dependent thickness of the amorphous layer that forms under ion bombardment, the ion-enhanced fluidity within that film, the magnitude of the stress being generated by the ion beam, and the strength of prompt atomic displacement mechanisms. Second, to further deepen our knowledge of surface dynamics, I have performed coherent X-ray studies of Ar⁺ bombardment of SiO₂ at the Advanced Photon Source (APS) for investigating the dynamics more profoundly than can be done with traditional time-resolved experiments. When using a focused ion beam, an inhomogeneous ripple motion was generated, this phenomenon reflected as an oscillatory behavior in the two-time and corresponding g₂(t) correlation functions. By fitting the oscillations in the g₂(t) correlation function, we have determined the surface ripple velocity on SiO₂ driven by Ar⁺ sputter erosion. Finally, to support the results of coherent X-ray experiments, simulations of growth models such as linear Kuramoto-Sivashinsky (KS) and Kardar-Parisi-Zhang (KPZ) have been carried out in order to compare the simulated temporal correlation functions of the scattered intensity with those obtained from the coherent x-ray scattering experiments.