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Self-assembled monolayers have been proven to be well-ordered and to give stable ultrathin films. They show a remarkably high diversity with respect to their functionalisation giving rise to many possible applications. This thesis is focused on the potential use of these molecular thin films in life sciences. The reproduction of a membrane-like environment with these tightly packed and organized unimolecular layers has led to important breakthroughs in their nanotechnological application as biomaterials. Their straightforward modification allows the chemical and physical properties of biological interfaces to be altered. In particular, Oligo(ethylene glycol) based alkanethiol self-assembled monolayers were intensively studied as biointerfaces for their ability to resist the non specific adsorption of proteins. The electrostatic repulsion which originates from these monolayers was seen as one of the possible factors causing this protein repulsion. On the other hand proteins adsorb on alkanethiol self-assembled monolayers. This can be partially attributed to an attractive hydrophobic interaction between the biomolecules and the surface. As a result of the understanding of these two driving forces which are relevant for non-specific protein adsorption/repulsion, novel self-assembling molecules were tailored in an attempt to adjust the adsorption of proteins at the SAM-liquid interface. This was conceivable with these newly designed SAMs since they allow a combination of these forces. We have chosen the ionic strength of the liquid environment as the external parameter which could act on the amount of adsorbed proteins because the electrostatic force created by oligo(ethylene glycol) groups depends on it. In addition to the synthesis of six new molecules, the preparation and characterisation of the novel self-assembled monolayers are reported in this thesis. The density of the monolayers was estimated by X-ray photoelectron spectroscopy and ellipsometry, and the wettability properties were studied by measuring the contact angle. The total force acting on proteins from the SAMs was studied with an atomic force microscope, equipped with a tip mimicking proteins, by measuring force-distance curves. An in-situ technique was investigated in order to study the influence of the variation of this total force on the quantity of adsorbed proteins by varying the ionic strength.

Note: / The soil-solution partitioning of dissolved organic carbon (DOC) withinmineral soil horizons is primarily controlled by processes of adsorption and desorption. These abiotic processes largely occur within a short equilibration time of seconds to minutes, which generally occur faster than microbial processes. To characterise the adsorption of DOC to mineral soils, I used the Langmuir adsorption isotherm, which holds several advantages to the commonly used linear initial mass (IM) isotherm. One advantage to using the Langmuir isotherm is anestimation of the maximum DOC adsorption capacity (Qmax). The Qmax estimates the number of remaining DOC binding sites available on the mineral soil particle surfaces. I modified the traditional Langmuir isotherm in order to estimate the DOC desorption potential of native soil organic matter (SOC).[...] / Le partitionnement entre les solutions de sols du carbone organiquedissous (COD) dans les horizons des sols minéraux est essentiellement contrôle par les processus d'adsorption et de désorption. Ces processus abiotiques se déroulent normalement dans un bref temps d'équilibration variant de quelques secondes a quelques minutes, ce qui est en général plus rapide que les processus microbiens. Pour caractériser Fadsorption de COD aux sols minéraux, nous avons utilise l'isotherme d'adsorption de Langmuir. Cette isotherme présente plusieurs avantages par rapport a Fisotherme de masses initiales (IM) linéaires couramment utilisée, en particulier F estimation de la capacité d'adsorption maximale du COD (Qmax). Le Qmax estime le nombre de sites de liaison de COD restants a la surface du sol minéral. Nous avons aussi modifie Fisotherme de Langmuir traditionnelle afin d'évaluer le potentiel de désorption de COD de la matière organique du sol indigène (MOS).[...]

The soil-solution partitioning of dissolved organic carbon (DOC) within mineral soil horizons is primarily controlled by processes of adsorption and desorption. These abiotic processes largely occur within a short equilibration time of seconds to minutes, which generally occur faster than microbial processes. To characterise the adsorption of DOC to mineral soils, I used the Langmuir adsorption isotherm, which holds several advantages to the commonly used linear initial mass (IM) isotherm. One advantage to using the Langmuir isotherm is an estimation of the maximum DOC adsorption capacity (Qmax). The Qmax estimates the number of remaining DOC binding sites available on the mineral soil particle surfaces. I modified the traditional Langmuir isotherm in order to estimate the DOC desorption potential of native soil organic matter (SOC). / Sorption characteristics were derived for a broad range of52 mineral soils collected from 17 soil profiles spanning across Canada from British Columbia to Quebec. Mineral horizons with the greatest Qmax included the Fe-enriched B horizons of acidic Podzols and Volcanic soils, followed by B horizons not enriched in Fe, followed by A and C horizons. Podzol B horizons were distinct from all other horizons due to significantly higher desorption potential. Soil properties predicting the adsorption characteristics of DOC also predicted the adsorption characteristics of dissolved organic nitrogen (DON). Adsorption of DOC and DON was tightly coupled (R 2 = 0.86), however the ratio of DOC:DON in the final equilibrium solution lowered for 48 out of 52 minerals horizons. These results suggest that DON may be slightly more mobile than DOC. / A short-term (32 day) incubation was perform to establish the fate of indigenous soil C, relative to newly adsorbed soil C to four mineral soils with different adsorption characteristics. Soil columns were leached periodically and sampled for DOC and CO2 production. Two Fe-enriched mineral horizons with high adsorption capacity released low amounts of old SOC, yet released almost all of the newly adsorbed SOC. In contrast, two B horizons without Fe-enrichment released greater amounts of old SOC, and retained a greater fraction of the newly adsorbed SOC than the Fe-enriched horizons. These results identify a contrast between the fate of indigenous and newly adsorbed SOC on mineral soils with differing Qmax. / The final component of this study examined changes to the molecular structure of DOC after equilibration with mineral soils. Multiple techniques were used to assess changes in the molecular composition of DOC, including the analysis of aromatic content by specific UV absorbance (SUVA) and fluorescence spectroscopy, analysis of molecular weight distribution (MWD) with high performance size exclusion chromatography (HPSEC) and functional group analysis with Fourier transform infra-red spectroscopy (FTIR). The solution phase DOC generally showed a reduced aromatic content, along with the removal of organic compounds with carboxyl groups. The MWD of DOC was reduced after equilibration to mineral soils, and the reduction in average molecular weight was related to the Qmax of mineral soils. / The various components of this thesis have contributed to the overall understanding of controls on the adsorption of DOC and DON species to mineral soils of the Canadian temperate and boreal forest.

Since 1982, the Si (111)-(7x7) surface has been extensively studied both theoretically and experimentally with the modern powerful tools of STM and Scanning Tunneling Spectroscopy (STS). In this work, a simple atomic orbital model for the Si (111)-(7x7) surface is developed to simulate the experimental results of STM and STS. Based on Tersoff-Hamann’s theory for the tunneling current, simulations of clean Si (111)-(7x7) constant-current images are presented. The direct, real-space simulated topographic images of the surface are compared to experimental results qualitatively and quantitatively. The simulation of spectroscopic imaging and normalized conductance spectra are also included. The adsorption of atomic hydrogen atoms onto the Si (111)-(7x7) surface is also simulated. / xiv, 146 leaves ; 29 cm.

The research presented in this thesis entailed an investigation of heavy metal uptake by Palmaria palmata, a red marine alga. The alga was dry and organically certified. The heavy metals of interest were those commonly found in the wastewaters of the printed wiring board industry, namely Cu2+Pb2+, Cd2+, Zn 2+ and Ni2+. The ultimate objective of the work was to determine whether or not the factors expected to influence the metal uptake to the greatest extent could be optimized within functional ranges, leading eventually to process design (beyond the scope of this thesis). These factors were pH, temperature, initial concentration of metal in aqueous solution, and contact time. A number of preliminary experiments were performed to establish a basis for the design of the optimization studies. / Although it was not possible to adequately define optimal regions of operation for the biosorption of heavy metals by Palmaria palmata , general trends were elucidated, and the limitations of the methodology used were clarified. (Abstract shortened by UMI.)

The adsorption behaviour of trace metals in soil may provide us with a way to more accurately predict and assess the toxicity of metals in the environment. This thesis reports efforts to apply surface complexation modeling to agricultural and forest soil and to relate model parameters to common soil properties. This study considered Ca, Cd, Cu, Pb and Zn but the methods here could be applied to other metals. In Chapter 2, the surface charge and adsorption behaviour of a set of Ap horizons was characterised using back-titration and batch adsorption techniques. With the objective of simplifying the application of the NICCA model to surface charge and cation adsorption in whole soils the parameters of the NICCA model were related to soil properties (Chapter 3). Four of the six surface charge parameters could be predicted from soil properties and this enabled me to reasonably predict the surface charge of a second group of soils from soil properties. These results suggest that it is possible to make reasonable predictions about the surface charge and adsorption behaviour of a given type of soil using some easily measurable soil properties and a set of generic NICCA adsorption parameters for that soil type. In Chapter 4 this idea is applied to the determination of lime requirement for the agricultural soils.

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The purpose of this study was to analyze the effect of fatty acid chain length and quantity on the bioavailability of calcium. Thirteen healthy subjects were randomly assigned to a series of 5 test meals containing varying types and levels of fat and calciumconsumed over a three week time period. The test meals included 10 grams MCT oil (MCT 10), 20 grams MCT oil (MCT 20), 10 grams beef fat (BT 10), 20 grams beef fat (BT 20), and calcium only (Ca). Calcium absorption was assessed using timed urine collections following a specified calcium load. Three day food records were obtained to assess typical nutrient intakes of the subjects coming into and during the study. MCT oil provided better absorption of the calcium supplement than did the beef tallow. A difference was also noted in the absorption of calcium based on the amount of fat consumed. A higher intake of MCT oil (10 g vs. 20 g) appeared to favor the absorption of calcium. Urine calcium excretion was significantly greater (p < .009) during the MCT oil treatments (MCT 10, MCT 20) compared to the beef fat treatments (BT 10, BT 20), suggesting reduced calcium absorption during the beef fat treatments. There were no differences in mean calcium excretion based on quantity of fat consumed ( 10 g vs. 20 g), nor any interaction between type of fat and amount. Tests for detecting differences between individual treatments indicated a significance difference (p < .05) in calcium excretion between MCT 20 and BT 10 treatments. Urine calcium excretion was corrected for body size using urine calcium/creatinine ratio (Ca/Cr). There was a significant time effect between the 0 - 2, 2 - 4 hour time periods (p < .005) and the various treatments for Ca/Cr. Though not significant, mean Ca/Cr was highest for the calcium treatment (0.42), compared to the MCT oil treatments (36, z of MCT 10 & MCT 20), and beef fat treatments (28, x of BT 10 & BT 20). The beef fat treatments significantly decreased the absorption of calcium compared to the MCT oil treatments. It appears that beef fat, when compared to the calcium only treatment, decreased calcium absorption. / Department of Home Economics