Rozprawy doktorskie: „Surface and interfaces”

1

Dahal, Arjun. "Surface Science Studies of Graphene Interfaces". Scholar Commons, 2015. http://scholarcommons.usf.edu/etd/5820.

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Interfaces between graphene and dissimilar materials are needed for making devices, but those interfaces also modify the graphene properties due to charge transfer and/or symmetry breaking. In this dissertation we investigate the technology of preparing graphene on different substrates and how the substrate influences the electronic properties of graphene. Synthesizing large area graphene on late transition metals by chemical vapor deposition is a promising approach for many applications of graphene. Among the transition metals, nickel has advantages because the good lattice match and strong interaction between graphene/Ni(111) enables the synthesis of a single domain of graphene on Ni(111). However, the nickel substrate alters the electronic structure of graphene due to substrate induced symmetry breaking and chemical interaction of the metal d-band with graphene. Similar chemical interactions are observed for other transition metals with a d-band close to the Fermi-level. On the other hand, graphene mainly physisorbs on transition metals with a lower lying d-band center. In this thesis we investigate the growth of graphene on nickel by vacuum chemical vapor deposition (CVD). In particular, we present our studies of graphene synthesis on Ni(111) substrates. We demonstrate the self-limiting monolayer of single domain of graphene can be grown on single crystal Ni(111). Our studies also show that selective twisted bilayer graphene can be grown by carbon segregation on Ni(111)-films. To modify the interaction between graphene and the nickel substrate we investigated the intercalation of tin. In the case of graphene physisorbed on weakly interacting metals, some charge doping of graphene occurs due to work function differences between graphene and the metal. Using x-ray photoemission spectroscopy (XPS) we correlate the charge doping of graphene on different metals with the C-1s binding energy. This study demonstrate that XPS can be used to determine the Fermi-level in graphene. While metal intercalation can alter the interaction with the substrate it does not avoid overlap of electronics states at the Fermi-level. Therefore a band gap material should be inserted between the graphene and the metal growth substrate (in this case Pt(111)). This is accomplished by oxidation of intercalated iron at elevated oxygen pressure. We demonstrate that a 2D-FeO layer can be formed in between graphene and the Pt(111) surface. We discuss the role of the 2D-FeO moiré-structure on the nanoscale electronic properties of graphene. To date good quality graphene can only be grown by CVD on late transition metals. To obtain graphene on other substrates the graphene can be transferred mechanically from a growth substrate to various other materials. We demonstrate that this transfer can also be achieved to tungsten, an early transition metal that easily forms a carbide. In our studies to avoid oxidation of the tungsten substrate and reaction of the graphene with the tungsten substrate under thermal treatment, protection of the W(110) surface with sulfur has been explored. For the integration of graphene into device architectures, graphene has to be interfaced with high-κ dielectrics. However, because of the inert nature of graphene, most high-κ do not wet graphene and thus preventing formation of contiguous dielectric layers. Yttrium oxide (Y2O3) has been demonstrated to be an exception and we characterized the growth of Y2O3 on various metal supported graphene and graphene transferred to SiO2. We showed that such a Y2O3 layer can also act as seeding layer for the growth of alumina, which is the preferred dielectric material in many applications. Finally, we investigate the charge doping of graphene in a metal/graphene/dielectric stack and find that the charge doping of graphene is a function of both the work function of the metal as well as the covering dielectric. Thus the dielectric layer can modify the charge doping of graphene at a metal contact.

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2

Purcell, Isabella Pauline. "Specular reflection from interfaces". Thesis, University of Oxford, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.386624.

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Hazell, Gavin D. A. "Surface scattering from soft matter at interfaces". Thesis, University of Bath, 2014. https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.642031.

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The aim of this work has been to make use of surface scattering techniques to study soft matter at interfaces. The work presented herein is composed of two distinct bodies of work. The first comprises a fundamental study of the physical and structural properties of Langmuir monolayers composed of sulfobetaine surfactants. Physiochemical properties of the films have been investigated through the use of Langmuir trough techniques. This has been used to support x-ray and neutron reflectometry data, from which structural parameters were derived. The second body of work involves attempts to find and/or characterize novel ways of aligning proteins at interfaces. Soluble proteins at lipid interfaces have been characterized in terms of their interactions with functionalized lipid monolayers. Specific interactions have been utilized to adsorb protein layers at the interface through interactions with His-tag chelating lipids within the monolayer. These have been characterized using neutron reflectometry and quartz crystal microbalance studies. Work has also been completed to design a suitable system for the adsorption of membrane proteins. This has involved aligning phospholipid bilayer nanodiscs at the lipid interface and subsequent characterization through neutron reflectometry.

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4

Wu, Liuming. "Surface complexation at calcium mineral-water interfaces". Doctoral thesis, Luleå, 1994. http://urn.kb.se/resolve?urn=urn:nbn:se:ltu:diva-25727.

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Surface reactions occurring at solid-water interfaces in calcium mineral-ligands systems have been studied. Both hydrous apatite and fluorite surfaces show clear amphoteric properties. An ion exchange process between lattice ions of F- on fluorite and OH- ions in bulk solution is discovered. The surface adsorption of Alizarin Red S and sodium oleate are determined. Surface chemical reaction models are established based on acidbase potentiometric titrations, solubility, adsorption and zeta-potential measurements in 0. 1 mol dm-3 ionic media at 25'C. Experimental data are evaluated using the computer program FITEQL assuming a constance capacitance model for the electric double layer. Surface complexes identities are obtained from FT-IR, FT-Raman, and UV/visible spectroscopy studies. A series of surface equilibrium constants in the system are presented. The correlation between surface complex formation and mineral flotation is discussed.
Godkänd; 1994; 20070429 (ysko)

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5

Maeda, Nobuo, i nobuo@engineering ucsb edu. "Phase Transitions of Long-Chain N-Alkanes at Interfaces". The Australian National University. Research School of Physical Sciences and Engineering, 2001. http://thesis.anu.edu.au./public/adt-ANU20011203.151921.

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An experimental study of phase transitions of long-chain n-alkanes induced by the effect of interfaces is described. ¶ The phase behaviour of long-chain n-alkanes (carbon number 14, 16, 17, 18) adsorbed at isolated mica surfaces and confined between two mica surfaces has been studied in the vicinity of and down to several degrees below the bulk melting points, Tm. Using the Surface Force Apparatus we have measured the thickness of alkane films adsorbed from vapour (0.97 [equal to or greater-than] p/p[subscript o] [equal to or greater-than] 0.997), studied capillary condensation transition, subsequent growth of capillary condensates between two surfaces, and phase transitions in both the adsorbed films and the condensates. By measuring the growth rate of the capillary condensates we have identified a transition in the lateral mobility of molecules in the adsorbed films on isolated mica surfaces. This transition to greater mobility occurs slightly above Tm for n-hexadecane, n-heptadecane and n-octadecane but several degrees below Tm for n-tetradecane, and is accompanied by a change in wetting behaviour and a measurable decrease in adsorbed film thickness for n-heptadecane and n-octadecane. Capillary condensates that form below Tm remain liquid, but may freeze if the degree of confinement is reduced by separation of the mica surfaces. An increase in the area of the liquid-vapour interface relative to that of the liquid-mica interface facilitates freezing in the case of the long-chain alkanes, which show surface freezing at the liquid-vapour interface. ¶ Although thermodynamic properties of the surface freezing transition have been rather well documented, the kinetics involved in formation of such ordered monolayers has so far received very little attention. We studied the surface tension of n-octadecane as a function of temperature in the vicinity of Tm, using the static Wilhelmy plate and the dynamic maximum bubble pressure methods. The two methods give different results on cooling paths, where nucleation of the surface ordered phase is involved, but agree on heating paths, where both methods measure properties of the equilibrium surface phase. On cooling paths, the surface of bubbles may supercool below the equilibrium surface freezing temperature. The onset of surface freezing is marked by a sharp drop in the surface tension. The transition is accompanied by an increased stability of the films resulting in longer bubble lifetimes at the liquid surface, which suggests that the mechanical properties of the surfaces change from liquid-like to solid-like. Our results suggest occurrence of supercooling of the monolayer itself.

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6

Li, Zhi Xin. "Neutron reflection from interfaces". Thesis, University of Oxford, 1996. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.320621.

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7

Johnson, Edward G. "Dynamics of interfaces and detergency". Thesis, Queen's University Belfast, 1997. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.361250.

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8

Bennett, Andrew Michael. "Properties, processes and surface chemistry at diamond interfaces". Thesis, University of Oxford, 2005. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.434867.

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9

Al-Bermany, Ehssan. "Polymer/graphene oxide nanocomposites : surface adsorption and interfaces". Thesis, University of Sheffield, 2017. http://etheses.whiterose.ac.uk/18510/.

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10

Iscimen, Mehmet. "Shearing Behavior Of Curved Interfaces". Thesis, Georgia Institute of Technology, 2004. http://hdl.handle.net/1853/7256.

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The frictional behavior of soil-construction material interfaces is of significant importance in geotechnical engineering applications such as retaining structures, pile foundations, geosynthetic liners, and trenchless technologies. Since most failures initiate and develop on the interfaces, special attention is required to predict the capacity of these weak planes in the particular application. Pipe-jacking and microtunneling technologies are being more widely used over the past decade and there is significant interest to predict the jacking forces and jacking distances achievable in order to achieve more efficient design and construction. This study focuses on the evaluation of the frictional characteristics and factors affecting the shear strength of pipe-soil interfaces. Eight different pipes made from fiber reinforced polymer (FRP), polycrete, steel, concrete, and vitrified clay were tested in the experimental program. For this purpose, a new apparatus was designed to conduct conventional interface direct shear testing on pipes of different curvature. This device allows coupons cut from actual conduits and pipes to be tested in the laboratory under controlled conditions. The apparatus includes a double-wall shear box, the inner wall of which is interchangeable to allow for testing against surfaces of different curvatures. By considering a narrow width section, the circular interface of pipes was approximated with a surface along the axial direction and the boundary is defined by the inner box. Roughness tests were performed using a stylus profilometer to quantify the surface characteristics of the individual pipes and relate these to the interface shear behavior. The surface topography showed different degrees of variability for the different pipes. To extend the range of roughness values tested and force the failure to occur in the particulate media adjacent to the interface, two artificial pipe surfaces were created using rough sandpapers. Interface shear tests were performed using the new apparatus with air-pluviated dense specimens of Ottawa 20/30 sand. Additional tests were performed using Atlanta blasting sand to evaluate the effect of particle angularity. The effect of normal stress and relative density were also examined. The interface strength was shown to increase with surface roughness and finally reach a constant value above a certain critical roughness value, which corresponded to the internal strength of the soil itself. This represented the failure location moving from the interface into the soil adjacent to the interface. Both the strength and the shearing mechanism were thus affected by the surface topography. It was also shown that the interface shear strength was affected by particle angularity, relative density and normal stress.

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11

Porter, Stephen Christopher. "Synthesis, surface characterization, and biointeraction studies of low-surface energy side-chain polyetherurethanes /". Thesis, Connect to this title online; UW restricted, 1999. http://hdl.handle.net/1773/9845.

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12

Larsericsdotter, Helén. "Macromolecules at Interfaces". Doctoral thesis, Uppsala University, Centre for Surface Biotechnology, 2004. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-4661.

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In this thesis, the structure and stability of globular proteins adsorbed onto nanometer-sized hydrophilic silica particles were investigated using differential scanning calorimetry (DSC), hydrogen/deuterium exchange (HDX), and mass spectrometry (MS). The adsorption process itself was characterized with fluorescence and absorption spectroscopy and surface plasmon resonance (SPR). The combination of these methods offered a unique insight into adsorption-induced changes within proteins related to their adsorption characteristics. DSC contributed with thermodynamic information on the overall structural stability within the protein population. HDX in combination with MS contributed information on the structure and stability of adsorbed proteins with focus on changes within the secondary structure elements. In order to increase the structural resolution in this part of the investigation, proteolysis was performed prior to the MS analyzing step. Knowledge on the protein adsorption process was utilized in a practical approach called ligand fishing. In this approach, SPR was used to monitor the chip-based affinity purification of a protein with MS used for protein identification.

Adsorption isotherms revealed that electrostatic interactions play an important role in the adsorption of proteins to hydrophilic surfaces. DSC investigation revealed that the thermal stability of proteins reduces with increasing electrostatic attraction between the protein and the surface and that this effect diminishes at higher surface coverage. The mass-increase due to exchange between protein hydrogen atoms and deuterium atoms in solution was investigated as a function of time. This gave insight into adsorption-induced changes in the structural stability of proteins. By combining DSC and HDX-MS, it was possible to differentiate between adsorption-induced changes in the secondary and tertiary structure. Additionally, if limited proteolysis was performed, the investigations gave insight into the orientation and protein segment specific changes in the stability of proteins adsorbed to silica surfaces. The adsorption of proteins to silica particles also provided the basis for a new experimental design that allows handling of minute amounts of proteins in a ligand fishing application, as used in the field of functional proteomics.

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13

Ong, Toon-Hui. "Vibrational spectroscopy of molecules at interfaces". Thesis, University of Cambridge, 1993. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.240827.

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14

Su, Tsueu-Ju. "Neutron and X-ray scattering from interfaces". Thesis, University of Oxford, 1996. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.319060.

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15

Took, Roger Kenton. "Surface interaction : separating direct manipulation interfaces from their applications". Thesis, University of York, 1990. http://etheses.whiterose.ac.uk/13997/.

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To promote both quality and economy in the production of applications and their interactive interfaces, it is desirable to delay their mutual binding. The later the binding, the more separable the interface from its application. An ideally separated interface can factor tasks from a range of applications, can provide a level of independence from hardware I/O devices, and can be responsive to end-user requirements. Current interface systems base their separation on two different abstractions. In linguistic architectures, for example User Interface Management Systems in the Seeheim model, the dialogue or syntax of interaction is abstracted in a separate notation. In agent architectures like Toolkits, interactive devices, at various levels of complexity, are abstracted into a class or call hierarchy. This Thesis identifies an essential feature of the popular notion of direct manipulation: directness requires that the same object be used both for output and input. In practice this compromises the separation of both dialogue and devices. In addition, dialogue cannot usefully be abstracted from its application functionality, while device abstraction reduces the designer's expressive control by binding presentation style to application semantics. This Thesis proposes an alternative separation, based on the abstraction of the medium of interaction, together with a dedicated user agent which allows direct manipulation of the medium. This interactive medium is called the surface. The Thesis proposes two new models for the surface, the first of which has been implemented as Presenter, the second of which is an ideal design permitting document quality interfaces. The major contribution of the Thesis is a precise specification of an architecture (UMA), whereby a separated surface can preserve directness without binding in application semantics, and at the same time an application can express its semantics on the surface without needing to manage all the details of interaction. Thus UMA partitions interaction into Surface Interaction, and deep interaction. Surface Interaction factors a large portion of the task of maintaining a highly manipulable interface, and brings the roles of user and application designer closer.

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16

Thapa, Nabin K. "Characterizing Liquid-Fluid Interfaces Using Surface Light Scattering Spectroscopy". Kent State University / OhioLINK, 2019. http://rave.ohiolink.edu/etdc/view?acc_num=kent1564059703319064.

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17

Noro, Hisato. "Surface processes at Ag/Fe and Fe/Ag interfaces". Thesis, University of Sussex, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.239113.

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18

Tissot, Héloïse. "Beyond the gap of pressure : XPS studies of interfaces at near ambient pressures". Thesis, Paris 6, 2014. http://www.theses.fr/2014PA066615/document.

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Dans de nombreux procédés technologiques, tels que la fabrication de matériaux pour la microélectronique, l’étude des réactions chimiques à une électrode, ou encore la catalyse… L’interface entre la surface d’un solide ou d’un liquide avec un liquide ou une phase gaz joue un rôle fondamental. De façon analogue, les sciences de l’environnement ainsi que celles du vivant intègrent dans leurs modèles la réactivité aux interfaces solide/ liquide ou liquide/ gaz.L’XPS est une technique parfaitement adaptée à l’étude des interfaces et a été largement utilisée pour l’analyse des surfaces de solides. Le principal avantage de l’XPS est sa grande sensibilité aux surfaces. En effet, en raison du faible libre parcours moyen des électrons dans un solide, uniquement les photoélectrons provenant de l’extrême surface (1 – 10 nm) peuvent échapper à celle-ci. Cependant, l’XPS est traditionnellement utilisée dans des conditions d’ultravide (UHV) et cela pour deux raisons. La première est que les analyseurs d’électrons sont construits pour fonctionner en UHV. La seconde est que les électrons doivent pouvoir atteindre l’analyseur, or leur libre parcours moyen est faible dans un gaz à haute pression. Par exemple, à une pression de 1 mbar, des électrons possédant une énergie de 100 eV vont parcourir 1 mm alors qu’ en UHV ils pourront atteindre jusqu’ à 105 m.Dans le but de rendre possible l’utilisation de l’XPS à des pressions plus élevées, quelques groupes autour du monde, dont le groupe de Berkeley (sous la direction de M. Salmeron at de H. Bluhm) et celui du Fritz Haber Institute à Berlin, ont élaborés un équipement permettant d’atteindre des pressions proche de l’ambiant (5 mbar). La construction d’un analyseur d’électron capable de fonctionner à des pressions de l’ordre du mbar, c’est-à-dire à des pressions 7 ordres de grandeur supérieures à l’UHV, a été une avancée à la fois conceptuelle et technologique. Un système de pompage différentiel permet de maintenir l’échantillon dans des conditions dites environnementales tout en maximisant le libre parcours moyen des électrons de façon à ce qu’ils atteignent l’analyseur. De plus, des tensions sont appliquées à des lentilles électrostatiques dans le but d’accélérer et de focaliser ces électrons.Un système similaire (Near Ambient Pressure XPS, NAP-XPS) a été installé sur la ligne TEMPO du synchrotron Soleil en février 2013, le premier temps de faisceau ayant eu lieu au mois de mai suivant. Durant ma thèse, deux projets différents ont été développés, tous les deux liés à l’étude d’interfaces avec l’utilisation de la NAP-XPS.Le premier projet traite des procédés utilisés en micro-electronique pour déposer de fines couches d’oxydes : le dépôt chimique en phase vapeur (CVD) et la déposition de couches atomiques (ALD). En particulier, des molécules de la famille des silanes sont utilisées pour fonctionnaliser des surfaces d’oxyde de silicium ou comme précurseur, combiné à un agent oxydant comme l’eau pour le dépôt de films mince d’oxyde de silicium. Cependant, les mécanismes réactionnels des silanes sur les surfaces de silicium n’ont jamais été étudiés par des techniques telles que la microscopie a effet tunnel (STM) ou l’XPS et l’on sait peu de choses concernant leur mécanisme de dissociation et l’adsorption des divers fragments sur la surface
In many processes or technological objects, such as coating deposition, advanced material processing for electronics, magnetic or optical devices, electrochemical processes at an electrode, sensors and catalysis, etc. the interface between a surface of a solid and a liquid or a gas phase, plays a prominent role. Analogously, environmental sciences and sciences of the Living integrate into their models chemical reactions taking place at solid/liquid or liquid/gas interfaces.XPS is a powerful technique for interface analysis and has been widely use in the case of solid surface. The main advantage of XPS is its sensitivity to the material surface. Indeed, due to the low electron mean free path of electrons in a solid, only the photoelectrons at the extreme outer surface (1-10 nm) can escape the sample. However, XPS has traditionally been conducted under ultra-high vacuum (UHV) conditions. UHV conditions are utilized for two reasons. First, the analyzers are designed to work under UHV conditions. Second, the electrons must reach the detector and their mean free path is short at high pressures. For example at a pressure of 1 mbar, 100 eV electrons will travel 1 mm while under UHV conditions, the mean free path increases to 105 m. UHV chambers (10-10 mbar) help maximize the mean free path so that a high number of electrons will reach the detector/analyzer and the signal/noise ratio will increase making it possible to analyze the spectrum produced. This constraint makes UHV the standard environment of X-ray Photoelectron Spectroscopy (XPS) experiments.In order to make possible the use of XPS on a larger pressure range, a few groups around the world have designed photoemission equipment that can be operated under ambient pressure (up to 5 mbar). The Berkeley group (M. Salmeron LBNL-Materials Sciences Division, H. Bluhm LBNL-Chemical Sciences Division), who pioneered this field, has two such setups installed at the Advanced Light Source. The Fritz Haber Institute has built a high pressure XPS based on the Berkeley prototype, installed at BESSY synchrotron (Berlin), since 2002. The building of Ambient Pressure XPS (APXPS) analyzers of the Berkeley type, able to be operated at pressures in the range of 1 mbar, about 7 orders of magnitude higher than the pressure limit of conventional UHV equipment is both a technological and conceptual breakthrough. Differential pumping stages allow the sample to remain at environmental pressures, while maximizing the mean free path of emitted electrons, so they can reach the detector. Additionally, voltages are applied to electrostatic lenses in the unit to accelerate and focus the electrons onto the focal plane of the electron energy analyzer. A similar system Near-Ambient Pressure XPS, NAP-XPS), described in details in chapter 1, was delivered in December 2012 and installed at TEMPO beamline in February 2013. The first beamtime occurred in May 2013. During my thesis that started in October 2011 two different projects were developed, both related to interface analysis using the NAP-XPS instrument

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19

Yang, Fuzi. "Optically excited surface polaritons using strongly absorbing media". Thesis, University of Exeter, 1991. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.279743.

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Szabo, Tamas. "Energy transfer at gas-liquid interface towards energetic materials /". Diss., Columbia, Mo. : University of Missouri-Columbia, 2007. http://hdl.handle.net/10355/4797.

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Thesis (Ph. D.)--University of Missouri-Columbia, 2007.
The entire dissertation/thesis text is included in the research.pdf file; the official abstract appears in the short.pdf file (which also appears in the research.pdf); a non-technical general description, or public abstract, appears in the public.pdf file. Title from title screen of research.pdf file (viewed on February 29, 2008) Vita. Includes bibliographical references.

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Arab, Arian. "Probing the Surface- and Interface-Sensitive Momentum-Resolved Electronic Structure of Advanced Quantum Materials and Interfaces". Diss., Temple University Libraries, 2019. http://cdm16002.contentdm.oclc.org/cdm/ref/collection/p245801coll10/id/547230.

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Physics
Ph.D.
In this dissertation, we used a combination of synchrotron-based x-ray spectroscopic techniques such as angle-resolved photoelectron spectroscopy (ARPES), soft x-ray ARPES, hard x-ray photoelectron spectroscopy (HAXPES), and soft x-ray absorption spectroscopy (XAS) to investigate momentum-resolved and angle-integrated electronic structure of advanced three- and two-dimensional materials and interfaces. The results from the experiments were compared to several types of state-of-the-art first-principles theoretical calculations. In the first part of this dissertation we investigated the effects of spin excitons on the surface states of samarium hexaboride (SmB6), which has gained a lot of interest since it was proposed to be a candidate topological Kondo insulator. Here, we utilized high-resolution (overall resolution of approximately 3 meV) angle-resolved and angle-integrated valence-band photoemission measurements at cryogenic temperatures (1.2 K and 20 K) to show evidence for a V-shap
Temple University--Theses

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Mao, B. W. "In-situ X-ray diffraction studies of electrochemical interfaces". Thesis, University of Southampton, 1987. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.378678.

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Barraud, Chloé. "Nanorhéologie de fluides complexes aux interfaces". Thesis, Université Grenoble Alpes (ComUE), 2016. http://www.theses.fr/2016GREAY011/document.

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Les liquides confinés présentent beaucoup de comportements fascinants, très différents de ceux qui sont observés dans leur volume. Le confinement peut induire un déplacement de l'équilibre des phases (par exemple de la transition liquide-vapeur, aussi appelé condensation capillaire), il peut modifier la température de transition vitreuses des polymères, ou bien imposer un ordre dans l'arrangement moléculaire du fluide. Les modifications des propriétés mécaniques des liquides aux interfaces sont particulièrement importantes au niveau des applications. Cependant au niveau de la compréhension, le simple cas des liquides newtoniens est toujours sujet à controverse, avec d'une part des simulations numériques montrant que la viscosité ne devrait pas être modifiée pour des confinements supérieurs à quelques tailles moléculaires, et d'autre part des expériences non unanimes, montrant parfois des modifications qualitatives des propriétés rhéologiques sous confinement. Récemment nous avons montré que les méthodes d'impédance hydrodynamique en géométrie sphère-plan constituent une méthode privilégiée, non-intrusive et non-ambigüe, pour aborder la nano-mécanique des liquides aux interfaces (1,2). S'agissant d'interphases, cad de couches fluides dont les propriétés sont modifiées par la proximité d'un solide, il est possible d'accéder à leur module sans contact, donc sans la perturbation apportée par une seconde surface. S'agissant de l'effet du confinement sur la rhéologie, nous avons montré que la déformation élastique à l'échelle du pico-mètre des surfaces confinantes, donne une forte modification de la rhéologie apparente du fluide, même en l'absence de tout effet intrinsèque. Le sujet de thèse vise à mettre en oeuvre les méthodes d'impédance hydrodynamique pour étudier la rhéologie de solutions de polymères confinés. On étudiera plus précisément deux systèmes modèles d'importance fondamentale aussi bien que pratique : les brosses de polymères greffés, dont les propriétés mécaniques sont un enjeu dans les applications de lubrification aussi bien que pour les écoulements biologiques, et les solutions de polymères hydro-solubles d'intérêt pour la récupération assistée du pétrole, en vue de comprendre les effets de fluidification sous confinement et de faire la part entre modification de la viscosité et couche de déplétion induite par l'écoulement. Au niveau instrumental, un des enjeux de la thèse sera de mettre en oeuvre les mesures d'impédance hydrodynamique sur deux types d'instruments complémentaires au niveau de l'échelle de la sonde: l'appareil de mesure de forces dynamique (SFA) du Liphy, et l'AFM à détection interférométrique développé à l'Institut Néel. Ces différentes échelles d'investigation devront permettre de préciser les propriétés moyennes mécaniques moyennes des liquides confinés et leurs gradients au voisinage de la paroi. Une perspective du travail sera de mettre en regard les propriétés mécaniques et rhéologiques intrinsèques des brosses polymères déterminées directement sur SFA ou AFM, avec leur propriétés fonctionnelles: propriétés de lubrification des contacts frottants, ou de modification des écoulements des dans micro-canaux. Ceci sera poursuivi sur la plateforme expérimentale mise en place par Lionel Bureau au Liphy : SFA de friction, systèmes micro-fluidiques à visée biomimétique (parois fonctionnalisées par des brosses polymères). L'enjeu sera alors de comprendre comment les propriétés mécaniques et rhéologiques des brosses déterminent celles des systèmes dans lesquels elles interviennent
Liquids confined present many fascinating behaviors very different from those observed in their volume. Confinement can induce a shift in the balance of phases (eg the liquid-vapor transition, also called capillary condensation), it can change the glass transition temperature of the polymer, or impose order on the molecular arrangement of fluid. The changes in the mechanical properties of liquid interfaces are particularly important in applications. However the level of understanding, the simple case of Newtonian liquids is still controversial, with one hand, numerical simulations show that the viscosity should not be changed for some higher molecular sizes containment, and secondly non-unanimous experiences, sometimes showing qualitative changes in rheological properties under confinement. Recently we have shown that the methods of hydrodynamic impedance sphere-plane geometry is a privileged, non-intrusive method and unambiguous, to discuss the mechanics of nano-liquid interfaces (1,2). As interphase, ie fluid layers whose properties are modified by the proximity of a solid, it is possible to accede their contactless module, so without the disturbance caused by a second surface.S As regards the effect of confinement on the rheology, we have shown that the elastic deformation across the pico meter of confining surfaces, gives a strong modification beyond apparent rheology of the fluid, even in the absence of any intrinsic effect. The thesis aims to implement the hydrodynamic impedance methods to study the rheology of polymer solutions confined. We specifically consider two models of fundamental importance as well as practical systems: brushes grafted polymer whose mechanical properties are an issue in lubrication applications as well as for biological flows and solutions of water-soluble polymers interest in enhanced oil recovery, in order to understand the effects of thinning containment and to distinguish between changes in viscosity and depletion layer induced by the flow. At the instrumental level, one of the challenges of the thesis is to implement the hydrodynamic impedance measurements on two complementary instruments at the level of the probe: the measuring dynamic power (SFA) of Liphy, and AFM interferometric detection developed at the Institut Néel. These different scales of investigation will help to clarify the medium average mechanical properties of liquids confined and their gradients near the wall. A view of work will be to look mechanical and rheological properties of polymer brushes intrinsic determined directly on SFA or AFM with their functional properties: lubricating properties of sliding contacts, or modification of the flow in microchannels. This will continue on the implementation by Lionel Bureau Liphy experimental platform: SFA friction advised biomimetic micro-fluidic systems (walls functionalized polymer brushes). The challenge will be to understand how the mechanical and rheological properties of brushes determine those systems in which they operate

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24

Lenne, Quentin. "Interfaces et nano-objets fonctionnels et biomimétiques pour l'électrocatalyse". Thesis, Rennes 1, 2021. http://www.theses.fr/2021REN1S143.

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Les travaux effectués dans le cadre de cette thèse se concentrent sur la fonctionnalisation covalente de nanoparticules métalliques par une monocouche de calix[4]arènes. L’activité catalytique de ces systèmes modifiés a ensuite été étudié lors de l’activation de petites molécules ressources comme le dioxygène, le méthanol, et le dioxyde de carbone
The work presented in this manuscript is focused on the surface functionalization of metallic nanoparticles with a covalently-bound monolayers of calix[4]arenes. The catalytic activity of these modified systems was then studied for the activation of small fuel molecules such as oxygen, methanol, and carbon dioxide

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Zhang, Xiaochun. "Design and characterization of biomolecule/semiconductor interfaces". Access to citation, abstract and download form provided by ProQuest Information and Learning Company; downloadable PDF file, 221 p, 2009. http://proquest.umi.com/pqdweb?did=1833646481&sid=4&Fmt=2&clientId=8331&RQT=309&VName=PQD.

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26

Dedinaite, Andra. "Surface force studies of association phenomena at solid-liquid interfaces". Doctoral thesis, KTH, Chemistry, 1999. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-2849.

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The main topics of this thesis, association phenomena inbulk and at solid-liquid interfaces in polar and non-polarmedia, were studied by a range of methods. Direct forcemeasurements employing the interferometric surface forceapparatus (SFA) was the chief technique. In addition, atomicforce microscopy (AFM), X-ray photoelectron spectroscopy (XPS),small angle neutron scattering (SANS), dynamic light scattering(DLS), turbidimetric and electrophoretic mobility measurementswere also applied. These techniques give complementaryinformation, and together they can provide a rather detailedpicture of the fairly complex systems studied.

The first system studied was designed to explore particleinteractions in non-polar media. It consisted of polar or,alternatively, non-polar surfaces immersed in a non-polarmedium, triolein, in some cases containing additives such asphospholipids, polyglycerol polyricinoleate (PGPR), and traceamounts of water. It was investigated how triolein mediates thesurface interactions and how these interactions are affected bythe presence of additives. Triolein adsorbs onto mica surfacesthus producing a barrier against flocculation of the particles.The additives mentioned interact with the surfaces and witheach other, thus altering the surface interactions. Water, forinstance, being strongly polar, preferentially adsorbs ontomica and disturbs the triolein ordering at the mica surfacescausing the barrier against flocculation to vanish. Owing tocapillary condensation of water, a strong adhesion between thesurfaces is instead developed. On the other hand, it could beshown that in the presence of phospholipids, the effect ofwater was opposite: long-range repulsive forces develop due toweakly adsorbed reversed phospholipid aggregates.

The second type of system studied contained cationicpolyelectrolytes and oppositely charged surfactants. Suchsystems occur in numerous technological processes: wastewatertreatment and ore recovery as well as laundry and body care.Polyelectrolytes and surfactants associate in bulk solution,and they also adsorb on surfaces. Thus, the relation betweenthe bulk properties of polyelectrolyte-surfactant mixtures andtheir properties at the solid-liquid interface is of greatscientific and industrial interest. The bulk properties ofpolyelectrolyte-surfactant aggregates were characterised byDLS, SANS, turbidimetry and electrophoretic mobilitymeasurements. It was concluded that to a certain extent theinterfacial properties of polyelectrolyte-surfactant aggregatescan be rationalised by considering their bulk properties.However, it was also shown that the presence of a surfaceaffects the association between polyelectrolytes andsurfactants. The chemical composition of adsorbed aggregates isdifferent from that of aggregates in solution, and, moreover,the structure of surface-bound polyelectrolyte-surfactantaggregates changes slowly with time.

Keywords:Triolein, phosphatidiylethanolamine,phospholipid, lecithin, capillary condensation, polyglycerolpolyricinoleate, aggregation, adsorption, surface forces,structural forces, mica, polar surface, non-polar surface,polyelectrolyte, surfactant, sodium dodecyl sulphate,polyelectrolyte-surfactant association, turbidity,electrophoretic mobility, AFM, SANS, DLS, SFA.

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Hahlin, Maria. "Electronic and Molecular Surface Structures of Dye-Sensitized TiO2 Interfaces". Doctoral thesis, Uppsala universitet, Yt- och gränsskiktsvetenskap, 2010. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-127166.

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The dye-sensitized solar cell is a promising solar cell technology. In these systems the key process for light to electricity conversion is molecular in nature and is initiated in dye molecules adsorbed at a semiconducting surface. This thesis focuses on the electronic and molecular surface structure of the dye/TiO2 interface, and the experimental results were obtained from surface sensitive X-ray based electron spectroscopic methods. Two families of dyes, triarylamine based organic dyes and ruthenium based inorganic dyes, were investigated. The effect of dye structural modications on the interfacial properties was studied, such as the surface concentrations, dye molecular surface orientation, molecular interactions, and energy level matching. Also, the impact of additional parameters such as the incorporation of coadsorbents and the solvents used for dye sensitization were studied and complementary photoelectrochemical characterization was used to demonstrate functional properties corresponding to changes in the molecular layers. The experiments provided information on how specic structural modications change the frontier electronic structure. The results also showed that the adsorption of the organic dye leads to submolecular electronic changes, and that the dye surface orientations in general favor effcient energy conversion. Moreover, effects of solvents and coadsorbents, on both energy level matching between the dye and the TiO2 substrate and the surfacemolecular structure were quantied.

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Bello, D. O. "The lubricant/surface topography interaction at press tool/blank interfaces". Thesis, Brunel University, 1985. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.481594.

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Rapisarda, Antonino. "Localized Surface Plasmon Resonance: Nanoscale Sensing for Processes at Interfaces". Doctoral thesis, Università di Catania, 2017. http://hdl.handle.net/10761/4022.

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This PhD thesis reports the use the emerging surface-sensitive optical technique of localized surface plasmon resonance (LSPR) to characterize the interaction of relevant classes of biomolecules, e.g. peptides, proteins, lipids and DNA strands, at solid-liquid interfaces, with an emphasis on deciphering kinetics and pathways of dynamic adsorption processes. LSPR-based biosensor exploits the high sensitivity of the plasmon frequency to refractive index changes confined to 5-30 nanometers around the metal nanoparticles deposited on the sensor surface to monitor in situ and in real time the interaction of unlabeled biological molecules skipping the misleading contribution from the bulk of solution affecting conventional optical technique, e.g. SPR and OWLS. In the present dissertation the advantages of applying this powerful technique are thoroughly demonstrated by investigating four case studies concerning relevant aspects for the biointerfaces science. The case of study 1 will involve the adsorption kinetics of single and binary solution of proteins onto model hydrophilic and hydrophobic surfaces. The analysis of the adsorption kinetics reveals that competitive adsorption occurs, at physiological pH 7.4 and relatively high ionic strength (NaCl 0.1 M), favoring the heavier protein (fibronectin, in our case), which is shown to adsorb faster and in larger amount than the lighter one (human serum albumin, in our case). The case of study 2 will discuss the DNA hybridization process for binary solutions of respectively perfectly matching (PM) and single base mismatching (MM) 93-mer ssDNA from KRAS codon 12, with a surface tethered probe complementary to the PM sequence. Sensitivity down to obtaining down to 10 nM and 13 nM, respectively for PM and MM were obtained, showing that the hybridization process occurs at a lower rate for MM with respect to PM target. The competitive hybridization was accounted for by an inhibition model, where the non-complementary sequences kinetically hinder the hybridization of the perfect matching sequences, owing to their above mentioned affinity constant differences for the same probe. The case of study 3 will cover the kinetics of phospholipid vesicle adsorption on silicon oxide surfaces as function of pH. Two different regimes have been observed for acidic and basic conditions. At low pH, vesicles adsorption showed one-step exponential kinetics. Moreover, no significantly variation of the adsorption rate was observed over the investigated pH range 3-6, suggesting the process is controlled by Van der Waals interactions and steric forces. At high pH, vesicles adsorb showing two-step kinetic. Furthermore, it was observed that the rate of the first step slows down linearly with the increasing of pH, suggesting that the process is primarily driven by vesicle-surface electrostatic repulsion. The case of study 4 will report preliminary results from the study of pH stimuli-responsive smart surfaces, formed by gold nanodisks array of an LSPR sensor chip decorated with Trichogin GA IV and two of its positively-charged analogs, i.e. Lipo-Lys and L20, in which four and eight Lysines positive charged residues have been introduced respectively. The surface-bound peptides exhibit reversible and rapid switching between conformations and can withstand several cycles of swelling and collapsing with no significant loss from the surfaces. Overall, the results here reported demonstrated the great potential of LSPR technique as a unique tool to monitor specific and non-specific biomolecular interactions at interfaces in application fields ranging from biosensing to materials science.

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Eftekharibafrooei, Ali. "Ultrafast Vibrational Spectroscopy and Dynamics of Water at Interfaces". Diss., Temple University Libraries, 2011. http://cdm16002.contentdm.oclc.org/cdm/ref/collection/p245801coll10/id/107351.

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Chemistry
Ph.D.
Over the past two decades, vibrational sum-frequency generation (VSFG) has been applied as a versatile technique for probing the structure and dynamics of molecules at surfaces and interfaces. The excellent surface specificity of the SFG allows for probing different kinds of liquid interfaces with no or negligible contribution from adjacent and much deeper bulk phase. VSFG spectroscopy has provided evidence that the structure of the water at interfaces is different from the bulk. With the ultrafast pulses, VSFG can also be used as a probe of ultrafast vibrational dynamics at interfaces. However, apart from a few pioneering studies, the extension of VSFG into time domain has not been explored extensively. Here VSFG is used as a probe of ultrafast vibrational dynamics of water at silica interfaces. Silica is an excellent model system for the solid phase where one can systematically vary the surface charge via bulk pH adjustment. The extension of the surface electric field, the interfacial thickness and surface accumulation of ions at a charged silica surface were studied using IR pump-VSFG probe spectroscopy. A vibrational lifetime (T1) of about 250 fs, similar to bulk H2O, was observed for the O-H stretch of H2O/silica interface when the silica surface is negatively charged. At the neutral surface, where the thickness of interfacial water is smaller than at the charged surface, the vibrational lifetime of O-H stretch becomes more than two times longer (T1~ 600 fs) due to the decreased number of neighboring water molecules, probed by SFG. The fast T1 at negatively charged surface begins to slow down by screening of the penetration of surface electric field via adding salt which suggests the primary reason for similar vibrational dynamics of water at charged interface with bulk water is the penetration of electric field. By decoupling of OH of HDO in D2O, a frequency dependent vibrational lifetime is observed with faster T1 at the red compared to the blue side of the hydrogen bond spectral region. This correlates with the redshift of the SFG spectra with increasing charged surface and is consistent with a theoretical model that relates the vibrational lifetime to the strength of the hydrogen bond network.
Temple University--Theses

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31

Rowe, S. J. "Adsorption studies of simple molecules on metalic, bimetalic and semiconductor interfaces". Thesis, University of Southampton, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.383911.

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Marana, Naiara Letícia [UNESP]. "Estudo computacional do óxido de zinco puro e dopado com metais de transição: bulk, superfícies, interfaces e nanotubos". Universidade Estadual Paulista (UNESP), 2017. http://hdl.handle.net/11449/150977.

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Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)
A química computacional tem se mostrado uma ferramenta muito útil no meio científico e tem sido cada vez mais utilizada na pesquisa de novos materiais. Dentre os muitos sistemas estudados com o auxílio da química computacional, destaca-se o óxido de zinco (ZnO), muito utilizado em diversos dispositivos eletrônicos tais como, sensores, células solares, diodos de emissão de luz UV e diodos a laser. À temperatura e pressão ambientes, a estrutura cristalina mais estável do ZnO é hexagonal do tipo wurtzita, na qual os átomos de zinco estão coordenados a quatro átomos de oxigênio. Devido a coordenação tetraédrica e falta de centro de simetria dessa estrutura, o ZnO apresenta propriedades piezoelétricas podendo ser aplicado em sensores piezoelétricos, por exemplo. Atualmente, existem muitos trabalhos científicos relacionados com o ZnO, porém o número de trabalhos teóricos em relação aos trabalhos experimentais ainda é pequeno. Neste sentido, este projeto teve como objetivo a análise das propriedades do ZnO em três morfologias diferentes, bulk, superfícies e nanotubos, aplicando as principais técnicas de modelagem computacional aplicada ao estado sólido tais como escolha do funcional de densidade e funções de base, otimização da geometria, dopagem por substituição de átomos, cálculo de constantes elásticas e piezoelétricas, simulação de pressão hidrostática aplicada a célula unitária, secção do bulk para gerar superfícies, substituição de átomos para formar interfaces, nanotubos e adsorção de moléculas nos nanotubos. Os cálculos foram realizados aplicando-se a Teoria do Funcional de Densidade, com o auxilio do programa CRYSTAL14, utilizando o funcional híbrido B3LYP, com o conjunto de funções de base all-electron. A metodologia aplicada conserva a periodicidade dos sistemas cristalinos (1D para nanotubos, 2D para superfícies ou 3D para bulk), em que os blocos de construção são compostos por células unitárias e podem ser replicados pelo operador de simetria. As análises topológicas foram realizadas aplicando-se a Teoria Quântica de átomos em Moléculas de Bader. Após a escolha do nível de teoria, as propriedades estruturais, eletrônicas, vibracionais, topológicas e constantes elásticas e piezoelétricas foram analisadas para o bulk. Partindo da estrutura otimizada, os átomos de zinco foram substituídos por Mn2+ e Al3+, simulando sistemas dopados. Paralelamente, foi realizado o estudo do comportamento das constantes elásticas e piezoelétricas em função da variação de pressão hidrostática, que mostrou a resposta piezoelétrica do ZnO aumenta em função da pressão. Após o estudo do bulk, as superfícies (101 ̅0), (112 ̅0) e (0001) foram analisadas e estudadas através de sua energia superficial, propriedades estruturais, eletrônicas e topológicas. A partir da monocamada da superfície (0001), os nanotubos armchair, zigzag e quiral foram gerados e estudados de acordo com sua obtenção, estabilidade e diferentes propriedades. A adsorção de moléculas de NH3 à parede dos nanotubos armchair e zigzag foi estudada onde foram investigadas as alterações nas propriedades decorrentes da adsorção, mostrando que os nanotubos de ZnO são possíveis de serem aplicados em sensores de gás amônia. Por fim, o estudo de sistemas com interface ZnO/GaN foram estudadas para as superfícies (101 ̅0) e (112 ̅0) e nanotubos armchair e zigzag. Ao final, concluiu-se que os sistemas de interface podem ser aplicados em LEDs, por exemplo, pois o controle de espessura e material pertencente à camada externa da interface leva a diferentes emissões no espectro eletromagnético, indo do UVA ao Verde. Com este estudo, pretendeu-se investigar o máximo das três morfologias do ZnO na fase wurtzita e sugerir algumas possíveis aplicações.
Computational chemistry has proved to be a very useful tool in the scientific field and has been increasingly used in the research of new materials. Among the many systems studied with the aid of computational chemistry, we highlight zinc oxide (ZnO), widely used in many electronic devices such as sensors, solar cells, UV light emitting diodes and laser diodes. At room temperature and pressure, the most stable crystalline structure of ZnO is hexagonal of the wurtzite type, in which the zinc atoms are coordinated to four oxygen atoms. Due to the tetrahedral coordination and lack of center of symmetry of this structure, the ZnO presents piezoelectric properties and can be applied in piezoelectric sensors, for example. Currently, there are many papers related to ZnO, however the number of theoretical articles in relation to the experimental works are still small. In this sense, this project aimed the analysis of ZnO properties in three different morphologies, bulk, surfaces and nanotubes, applying the main techniques of computational modeling to solid state such as the choice of density functional and basic functions, optimization of geometry, doping by atom replacement, calculation of elastic and piezoelectric constants, hydrostatic pressure simulation applied to unit cell, bulk section to generate surfaces, replacement of atoms to form interfaces, nanotubes and adsorption of molecules in nanotubes. The calculations were performed applying the Density Functional Theory, with the help of the CRYSTAL14 program, using the hybrid function B3LYP, with the set of all-electron base functions. The applied methodology preserves the periodicity of the crystalline systems (1D for nanotubes, 2D for surfaces or 3D for bulk), in which the building blocks are composed of unit cells and can be replicated by the symmetry operator. The topological reviews were performed applying the Quantum Theory of atoms in Bader's Molecules. After choosing the level of theory, the structural, electronic, vibrational, topological and elastic and piezoelectric constants were analyzed for bulk. From the optimized structure, the zinc atoms were replaced by Mn2+ and Al3+, simulating doped systems. In parallel, a study of the behavior of the elastic and piezoelectric constants was conducted due to the hydrostatic pressure variation, which showed that the piezoelectric response of ZnO increases according to the pressure. After the bulk study, the surfaces (101 ̅0), (112 ̅0) and (0001) were analyzed and studied through their surface energy, structural, electronic and topological properties. From the surface monolayer (0001), the armchair, zigzag and chiral nanotubes were generated and studied according to their obtainment, stability and different properties. The adsorption of NH3 molecules to the wall of the armchair and zigzag nanotubes was studied and an investigation of the changes in the adsorption properties was carried out, showing that ZnO nanotubes are possible to be applied in ammonia gas sensors. Finally, the study of systems with ZnO/GaN interface was conducted for the surfaces (101 ̅0) and (112 ̅0), and armchair and zigzag nanotubes. At the end, it was concluded that the interface systems can be applied in LEDs, for example, because the control of thickness and material belonging to the outer layer of the interface leads to different emissions in the electromagnetic spectrum, going from UVA to green. This study aimed to investigate the maximum of three ZnO morphologies in the wurtzite phase and to suggest some possible applications.
FAPESP: 2013/19713-7
FAPESP: 2016/07954-8

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33

Tinel, Liselotte. "Des réactions photochimiques aux interfaces atmosphériques". Thesis, Lyon 1, 2015. http://www.theses.fr/2015LYO10263/document.

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Les travaux présentés dans cette thèse portent premièrement sur la caractérisation de nouveaux photosensibilisateurs par des méthodes spectroscopiques. Ainsi les cinétiques de la réaction d'oxydation entre deux photosensibilisateurs à l'état triplet, imidazole-2-carboxaldehyde et 6-carboxypterine, et trois halogénures ont été déterminées par photolyse laser. La réactivité de l'état singulet de la 6- carboxypterine avec les halogénures et quatre acides organiques a été étudiée par fluorimétrie. Ces photosensibilisateurs sont relevants pour la photochimie à la surface de l'océan, mais également à la surface des particules atmosphériques. Les réactions mises en évidence mènent à la formation d'espèces radicalaires très réactives, influençant ainsi la composition de la phase condensée et gazeuse de l'environnement marin. La suite de cette étude s'est focalisée sur l'analyse des produits formés à partir de processus photo-induites à interface air-eau en présence d'une microcouche de surface d'un organique, utilisant deux organiques différents, l'octanol et l'acide nonanoique. En présence d'un photosensibilisateur et de lumière UVA, les changements en phase gaz ont été suivi par SRI-ToF-MS en ligne et en phase condensée par UPLC-(ESI)-HRMS. Ainsi on a démontré que la photochimie à la surface mène à la formation de produits fonctionnalisés et insaturés initiée par une abstraction d'hydrogène sur l'organique surfactant. Ces produits, observés en phase condensée et gazeuse, ont le potentiel de contribuer à la formation d'aérosols. Etonnamment, des produits ont également été observés dans les deux phases sans l'ajout d'un photosensibilisateur et montrant une activité photochimique de l'acide nonanoique seul à l'interface air-eau. Les mécanismes potentiels et les conséquences environnementales sont discutés
The works presented in this thesis concern firstly the characterization of two new photosensitizers by spectroscopic methods. This way the kinetics of the oxidation reaction between the triplet state of the photosensitizers, imidazole-2-carboxaldehyde and 6-carboxypterin, and three halides have been determined by laser flash photolysis. Also, the reactivity of the singlet state of 6-carboxypterin with halides and four organic acids has been studied by static fluorimetry. These photosensitizers are relevant for the photochemistry at the surface of the ocean, but also at the surface of atmospheric particles. The reactions evidenced by these studies lead to the formation of very reactive radical species influencing the composition of the condensed and gas phase of the marine environment. This study then focalized on the analysis of the products formed at the organic coated air-water interface through photo-induced processes. Two different organics were used as surfactants, octanol and nonanoic acid. In the presence of a photosensitizer and UVA light, the changes in the gas phase were monitored online by SRI-ToF-MS and in the condensed bulk phase by UPLC-(ESI)-HRMS offline analysis. These analysis showed that photochemical reactions at the interface lead to the formation of functionalized and unsaturated compounds initiated by a hydrogen abstraction on the organic surfactant. These products, observed in the condensed and gas phase have the potential to contribute to the formation of aerosols. Surprisingly, some of these products were also observed in the two phases without the presence of a photosensitizer, bringing into evidence a photochemistry of nonanoic acid at the air-water interface. Potential formation mechanisms of the products and environmental consequences are discussed

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Srour, Rafif K. "Metal-surface reactions in mixed aqueous organic solvents". Morgantown, W. Va. : [West Virginia University Libraries], 2004. https://etd.wvu.edu/etd/controller.jsp?moduleName=documentdata&jsp%5FetdId=3582.

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Thesis (Ph. D.)--West Virginia University, 2004.
Title from document title page. Document formatted into pages; contains xix, 140 p. : ill. Includes abstract. Includes bibliographical references (p. 133-140).

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Nunnery, Grady A. "The influence of surface curvature on polymer behavior at inorganic surfaces". Diss., Georgia Institute of Technology, 2010. http://hdl.handle.net/1853/33929.

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Nanoscale surfaces were examined in order to determine the influence of surface curvature on polymer behavior at polymer-ceramic interfaces, as well as the influence of nanoparticles in cellulosic media. Poly(methyl methacrylate) and block copolymers thereof were adsorbed onto porous alumina substrates of various pore sizes in order to determine how polymer and copolymer adsorption behavior at nanoscale surfaces differs from adsorption onto flat surfaces. It was determined that chain density on concave surfaces dramatically decreases as curvature increases in much the same way that it does on convex surfaces (e.g. on the surface of nanoparticles), and physical models are provided to explain this similarity. Diblock copolymer adsorption is observed to vary dramatically with solvent quality and block asymmetry and can be correlated with the surface curvature very similarly to the adsorptive behavior of homopolymers on those same surfaces. The addition of nanoparticles to cellulosic media was investigated as a means to significantly modify the properties of cellulosic composites with minimal additions of nanoparticles. Although cellulose is among the most abundant polymers on earth, its primary uses are limited to bulk commodity goods, such as paper and textiles. This work demonstrates a simple means to control cellulosic fluid viscosity, thereby increasing the versatility of these biopolymers in additional applications with higher value-added potential. The formation of iron-cellulosic nanocomposites by the in-situ thermolysis of metal carbonyls to form metallic nanoparticles was performed and was analyzed by viscometry among other techniques. It was determined that the nanocomposites that were formed exhibited significantly increased viscosity, up to the point of gelation. Additionally, an introduction to the expansive field of nanocomposites is provided, including how and why composite properties change abruptly as filler size approaches the nanoscale. An extensive background on this diverse field as it relates to the current work is provided with an emphasis on cellulosic nanocomposites and the dependence of curvature on polymer-surface interactions. A detailed account of the experimental work relevant to this work is provided, including materials and characterization methods. Future work is proposed for both cellulosic nanocomposites as well as for curvature-dependent polymer adsorption. Finally, conclusions are drawn from the entire work and its implications to the greater field of nanocomposites.

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36

Kjellin, Mikael. "Structure-Property Relationships of Surfactants at Interfaces and Polyelectrolyte-Surfactant Aggregates". Doctoral thesis, KTH, Chemistry, 2002. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-3299.

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The first part of this thesis is concerned with thestructure-property relationships in nonionic surfactantsystems. The main aim was to investigate how the surfactantstructure influences the adsorption at interfaces andinteractions between surfactant coated interfaces.Particularly, the effect of the structure of the surfactantheadgroups was investigated. These were sugar-based headgroupwith varying size and flexibility and poly(ethylene oxide)based headgroups with or without an additional amide or estergroup. The hydrophobic part of the surfactant consisted mostlyof straight alkyl chains, except for one type of poly(ethyleneoxide) based surfactant with a dehydroabietic hydrophobe.

The main technique that was used is the surface forcetechnique, with which the forces acting between two adsorbedsurfactant layers on hydrophilic or hydrophobic surfaces can bemeasured. These forces are important for e.g. the stability ofdispersions. The hydrophilic surfaces employed were glass andmica, whereas the hydrophobic surfaces were silanized glass andhydrophobized mica. The adsorption behavior on hydrophilicsurfaces is highly dependent on the type of headgroup andsurface, whereas similar results were obtained on the two typesof hydrophobic surfaces. To better understand how the surfaceforces are affected by the surfactant structure, measurementsof adsorbed amount and theoretical mean-field latticecalculations were carried out. The results show that the sugarsurfactant layers and poly(ethylene oxide) surfactant layersgive rise to very different surface forces, but that the forcesare more similar within each group. The structure-propertyrelationships for many other physical properties have beenstudied as well. These include equilibrium and dynamicadsorption at the liquid-vapor interface, micelle size, micelledynamics, and wetting.

The second part in this thesis is about the aggregationbetween cationic polyelectrolytes and an anionic surfactant.The surface force technique was used to study the adsorption ofa low charged cationic polyelectrolyte on mica, and theaggregation between the adsorbed polyelectrolyte with theanionic surfactant. The aggregation in bulk was studied withturbidimetry, small angle neutron scattering (SANS), and smallangle x-ray scattering (SAXS). An internal hexagonal aggregatestructure was found for some of the bulk aggregates.

Keywords:nonionic surfactant, sugar surfactant,poly(ethylene oxide), amide, ester, polyelectrolyte, SDS,hydrophobic surface, glass surface, mica, adsorption,aggregation, micelle size, surface forces, wetting, dynamicsurface tension, NMR, TRFQ, SANS, SAXS, mean-field latticecalculations.

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37

Souharce, Grégoire. "Génération de surface nanostructurées par le contrôle des interactions aux interfaces". Phd thesis, INSA de Lyon, 2012. http://tel.archives-ouvertes.fr/tel-00845841.

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La génération de surfaces présentant des nanostructurations de surface variées et modulables est l'objectif principal de ce travail. L'auto-assemblage de copolymères à bloc ou de nanoparticules d'or a été privilégié, et nécessite pour se faire de moduler finement les interactions aux interfaces substrat/ matériaux déposés. Dans une première partie, un dispositif expérimental de greffage de silane alkyle en voie vapeur est décrit. Cette technique de greffage permet d'aboutir à des surfaces fonctionnalisées soit de façon homogène, soit de façon graduelle et ce, avec un ou deux silanes (substrat respectivement mono ou bi-composant). La robustesse, la simplicité et la flexibilité de notre procédé ont été démontrés par des caractérisations physico-chimique (mesure des propriétés de mouillabilité), chimique (spectroscopie de photoélectrons X) ainsi que par analyse topographique (microscopie à force atomique). Dans une deuxième partie, l'influence des interactions aux interfaces substrat / film sur l'auto-assemblage de copolymères à bloc PS-b-PMMA a été mise en évidence par AFM. A partir des substrats de silicium homogènes en énergie de surface, il a été possible de moduler la nanostructuration sur différents échantillons et à partir des surfaces fonctionnalisées graduellement, cette variation de nanostructuration a pu être obtenue sur un même substrat. Par l'utilisation de copolymère à bloc PS-b-PI, il est par ailleurs possible de générer des films nanostructurés sans préfonctionnalisation du substrat, sans recuit et ce quelle que soit l'épaisseur du film. Dans une troisième partie, l'influence des interactions aux interfaces sur l'assemblage capillaire/convectif dirigé de nanoparticules d'or a été démontré par microscopie à champ sombre. La nature chimique et la densité de greffage des silanes ainsi que la dimension des échantillons ont été modulées pour mettre en évidence le rôle de ces paramètres sur l'assemblage de ces particules. Cette étude montre que les interactions aux interfaces contrôlent l'assemblage des entités chimiques organiques et inorganiques et donc la nanostructuration de surface qui en résulte.

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Bhattarai, Bishal. "Wetting properties of structured interfaces composed of surface-attached spherical nanoparticles". Wright State University / OhioLINK, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=wright1544817024854422.

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39

Juang, Agnes Okumura Mitchio Lewis Nathan Saul. "Effects of surface modification on charge-carrier dynamics at semiconductor interfaces /". Diss., Pasadena, Calif. : California Institute of Technology, 2003. http://resolver.caltech.edu/CaltechETD:etd-08062002-192958.

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40

Manesse, Maël. "Développement de nouvelles interfaces plasmoniques appliquées à la biodétection". Grenoble INPG, 2009. http://www.theses.fr/2009INPG0056.

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L'utilisation de techniques de détection sans marquage telles que les méthodes basées sur la résonance de plasmons de surface (SPR) et l'électrochimie représentent un enjeu très important dans le développement des capteurs miniaturisés. Dans ce travail de thèse, de nouvelles interfaces adaptées aux études SPR-électrochimique ont été développées. Ces interfaces sont formées en déposant un film mince d'oxyde sur des substrats Titane/Or (Ti/Au) classiquement utilisés en SPR. Différents types d'interfaces hybrides ont été développées, comme Ti/Au/SiOx (oxyde de silicium), Ti/Au/SnO2:Sb (oxyde d'étain dopé antimoine) et Ti/Ag/SnO2:Sb. La caractérisation de ces nouvelles couches a été menée par électrochimie, résonance de plasmons de surface et spectroscopie de photoélectrons X (XPS). Différentes étapes de chimie de surface ont été étudiées sur ces interfaces afin de montrer la possibilité de greffer de manière covalente des biomolécules comme l'ADN sur le film d'oxyde
In this research work, new interfaces adapted for surface plasmon resonance (SPR) and electrochemical studies were developed for biosensing applications. These interfaces are formed by depositing thin oxide films on Titanium/Gold (Ti/Au) substrates, classically used in SPR. Different types of hybrid interfaces were formed, such as Ti/Au/SiOx (silicon oxide), Ti/AU/SnO2:Sb (antimony doped tin oxide), and Ti/Ag/SnO2:Sb. These new interfaces were characterized by SPR,, elechemistry and X-ray photoelectron spectroscopy (XPS). Different surfaéce chemistry approaches were investigated with the aim to covalenty link biomolecules to the oxide surface. Finally, we show the possibility of forming o localized surface plasmon resonance (L-SPR) sensing platform. It is based on the integration of gold nanoparticles into a biopolymer matrix

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41

Benusiglio, Adrien. "Indiscrétions aux interfaces". Phd thesis, Ecole Polytechnique X, 2013. http://pastel.archives-ouvertes.fr/pastel-00860739.

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Un corps qui se déplace dans l'eau y laisse des empreintes qui deviennent visibles s'il se rapproche de la surface. Dans cette thèse, nous étudions expérimentalement et théoriquement trois types différents d'empreintes, les "explosives", les "tourbillonnantes" et les "ondulantes". Les premières sont créées par des explosions à la surface de l'eau et engendrent des cavités dont on étudie la taille maximale et à la dynamique. Contrairement aux cavités d'impact, ces cavités explosives se caractérisent par une ouverture isotrope (cavité hémisphérique) et une fermeture anisotrope qui donne lieu à la formation d'un jet central. Si l'explosion est confinée par un cylindre ouvert de "petit" diamètre, on montre que la cavité se développe dans le cylindre mais n'en sort jamais, quelle que soit l'énergie de l'explosion. Pour les empreintes "tourbillonnantes", on étudie l'impact d'un tourbillon toroïdal sur une surface libre avec une attention particulière pour la taille maximale de la région perturbée et la durée de l'interaction. On montre que la nature chimique de l'interface joue un rôle crucial sur l'interaction: dans l'eau, celle-ci engendre des tourbillons secondaires qui limitent à deux diamètres la taille de la zone perturbée. Ces tourbillons sont supprimés dans l'éthanol et l'interaction s'y poursuit sur des dizaines de diamètres. La troisième partie "ondulante" porte sur la trainée de vague de sphères immergées. Expérimentalement, nous observons un fort écart entre les modèles théoriques classiques et la mesure, dans la gamme de profondeur et de vitesse pour laquelle celle-ci est importante. En étudiant le sillage de surface formé par les sphères, on montre que la saturation en amplitude de celui-ci est à l'origine de cet écart.

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42

Morgan, S. J. "An experimental study of the vanadium and calcium fluoride/silicon (111) interfaces". Thesis, Bucks New University, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.234711.

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43

Vessely, Christina Regina. "Effects of solution parameters on the adsorption of proteins at interfaces /". Connect to full text via ProQuest. IP filtered, 2006.

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Thesis (Ph.D. in Pharmaceutical Sciences) -- University of Colorado at Denver and Health Sciences Center, 2006.
Typescript. Includes bibliographical references (leaves 159-173). Free to UCDHSC affiliates. Online version available via ProQuest Digital Dissertations;

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44

Bourdoucen, Hadj. "Etude des surfaces d'InP et des interfaces InP-isolant par photoluminescence". Grenoble 2 : ANRT, 1987. http://catalogue.bnf.fr/ark:/12148/cb376033378.

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45

Guzha, Alphonce Chenjerayi. "Integrating Surface and Sub Surface Flow Models of Different Spatial and Temporal Scales Using Potential Coupling Interfaces". DigitalCommons@USU, 2008. https://digitalcommons.usu.edu/etd/50.

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The main objective of this research was to develop and utilize a coupled surface water groundwater model to simulate hydrological responses of watersheds. This was achieved by coupling the U.S. Geological Survey (USGS) groundwater flow model, MODFLOW, and the rainfall runoff model, TOPMODEL, in one case study and coupling MODFLOW with a networked version of TOPMODEL called TOPNET in another case study. The model coupling was achieved using the InCouple approach, which utilizes Potential Coupling Interfaces (PCIs) that are abstractions from model flow diagrams that expose only those aspects of a model relevant to coupling. Coupling the rainfall-runoff models to MODFLOW involved development of a routine relating the spatial discretization of MODFLOW to TOPMODEL and similarly MODFLOW to TOPNET and development of a feedback scheme where groundwater and surface water interact in the soil zone. The key coupling concept was replacing the wetness index-based depth-to-water table concept of TOPMODEL with the groundwater heads simulated by MODFLOW. In the MODFLOW-TOPMODEL coupling, using data for the Tenmile Creek watershed, for the period, 1968 to 1972, it was concluded that the coupled model was able to continuously simulate the stream flow. However, the coupled model under predicted stream flow and did not agree well with observations in a point wise comparison. A mean coefficient of efficiency of 0.54 was obtained between simulated and measured stream flow. Only 24% of received precipitation was observed as baseflow and this shows that there is limited interaction between surface water and groundwater in the watershed. It was demonstrated using the coupled model that the lateral flow processes and the interactions between groundwater and surface water have a major importance for the water balance. For the Big Darby watershed, for the period 1992 to 2000, the coupled model adequately predicts the stream and groundwater flow distribution in the watershed. After model calibration, simulated groundwater showed the greatest residual variance, attributed to model error and uncertainty in model parameters. Model fit efficiencies of 0.61 and 0.69 were obtained for simulating stream flow measured at two gaging stations. The overall watershed hydrologic budget also showed small mass balance errors using the coupled model. However, the study also shows the need for further research in regard to constraining the groundwater recharge parameter which links the models.

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46

Monga, Tanya. "Surface stress at the solid-liquid interface : alkanethiol monolayers on gold". Thesis, McGill University, 2006. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=101628.

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Defective alkanethiol monolayers were studied as a model system to understand the stress changes observed in microcantilever-based DNA hybridization experiments. An exponential relationship between defect density and surface stress was found by performing simultaneous electrochemical/stress-sensing experiments. Microcantilevers with a range of defective alkylthiol self assembled monolayers were prepared and stress change/electrochemical data were collected in perchlorate, chloride, and bromide-containing electrolytes. Defects were probed using a ferrocene-thiol labeling technique which provides quantitative measurement of defect area. Using defects and solutions containing charge transferring adsorbates is suggested as a method for enhancing the surface stress signals in cantilever sensor systems. The best response from this study was obtained in bromide, as its exponential function had the sharpest increase with defect density.

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47

Blomfield, Christopher James. "Study of surface modifications for improved selected metal (II-VI) semiconductor based devices". Thesis, Sheffield Hallam University, 1995. http://shura.shu.ac.uk/19362/.

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Metal-semiconductor contacts are of fundamental importance to the operation of all semiconductor devices. There are many competing theories of Schottky barrier formation but as yet no quantitative predictive model exists to adequately explain metal-semiconductor interfaces. The II-VI compound semiconductors CdTe, CdS and ZnSe have recently come to the fore with the advent of high efficiency photovoltaic cells and short wavelength light emitters. Major problems still exist however in forming metal contacts to these materials with the desired properties. This work presents results which make a significant contribution to the theory of metal/II-VI interface behaviour in terms of Schottky barriers to n-type CdTe, CdS and ZnSe. Predominantly aqueous based wet chemical etchants were applied to the surfaces of CdTe, CdS and ZnSe which were subsequently characterised by X-ray photoelectron spectroscopy. The ionic nature of these II-VI compounds meant that they behaved as insoluble salts of strong bases and weak acids. Acid etchants induced a stoichiometric excess of semiconductor anion at the surface which appeared to be predominantly in the elemental or hydrogenated state. Alkaline etchants conversely induced a stoichiometric excess of semiconductor cation at the surface which appeared to be in an oxidised state. Metal contacts were vacuum-evaporated onto these etched surfaces and characterised by current-voltage and capacitance-voltage techniques. The surface preparation was found to have a clear influence upon the electrical properties of Schottky barriers formed to etched surfaces. Reducing the native surface oxide produced near ideal Schottky diodes. An extended study of Au, Ag and Sb contacts to [mathematical formula] substrates again revealed the formation of several discrete Schottky barriers largely independent of the metal used; for [mathematical formula]. Deep levels measured within this study and those reported in the literature led to the conclusion that Fermi level pinning by native defects is a dominant mechanism in Schottky barrier formation in these systems.

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48

Bouali, Bachir. "Contribution à l'étude des phénomènes de mouillage pour la caractérisation des surfaces et interfaces : maîtrise de la physico-chimie et de la morphologie des surfaces pour régler les propriétés fonctionnelles des interfaces : applications industrielles". Lyon 1, 1998. http://www.theses.fr/1998LYO10132.

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La maitrise du comportement d'une surface est un element important qui intervient dans divers processus technologiques et biologiques tels que la lubrification, l'usure, l'adhesion, la glisse, la detergence, l'adsorption des proteines l'etude des phenomenes a l'interface est determinante pour l'optimisation de ces processus. Le mouillage peut etre considere comme un outil d'investigation pour etudier les proprietes d'une telle interface et notamment les proprietes d'usage caracteristiques de chaque domaine d'application. Dans le present travail, nous avons exploite differentes approches de la mouillabilite aussi bien pour la description du liquide mouillant que du solide mouille. Dans un premier temps, nous nous sommes attaches a decrire, les interactions moleculaires a l'interface liquide - solide et a evaluer la pertinence les differents modeles proposes pour estimer l'energie de surface du solide. Nous avons ensuite examine les relations entre la topographie de la surface solide et les angles de contact a l'aide d'une approche pluridisciplinaire originale faisant intervenir les aspects morphologiques et physico-chimiques de cette surface. La partie liquide de l'interface a ete prise en compte en etudiant le comportement au mouillage de differents liquides sur des surfaces solides connues et bien caracterisees. Enfin, nous avons etudie l'hysteresis de mouillage a partir du comportement dynamique de gouttes de liquide decrochant sur une surface inclinable. L'ensemble des travaux exposes constitue une contribution a la caracterisation de l'interface liquide-solide et propose une methodologie generale d'approche de cette interface.

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Charest, Joseph Leo. "Topographic and chemical patterning of cell-surface interfaces to influence cellular functions". Diss., Atlanta, Ga. : Georgia Institute of Technology, 2007. http://hdl.handle.net/1853/24621.

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Thesis (Ph. D.)--Mechanical Engineering, Georgia Institute of Technology, 2007.
Committee Chair: Dr. William P. King; Committee Member: Dr. Andres J. Garcia; Committee Member: Dr. F. Levent Degertekin; Committee Member: Dr. Hang Lu; Committee Member: Dr. Todd C. McDevitt.

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50

Robb, David Andrew. "An investigation of the nature of the interaction of dicyandiamide cured epoxy resin adhesives with aluminium substrates, using model compounds". Thesis, University of Strathclyde, 2001. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.366906.

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