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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

Growth and characterization of graphene on 4H-SiC(0001)

Ektarawong, Annop January 2012 (has links)
Thermal annealing 4H-SiC(0001) substrates to produce epitaxial graphene on Si-terminated SiC was performed using five different procedures, i.e. direct and indirect current heating at different based pressures and a temperature of about 1300 . The aim is to study the effects of graphene growth under different conditions and also to produce large homogeneous graphene. To investigate the prepared samples, two surface analytical techniques, i.e. low energy electron microscopy (LEEM) and photoelectron spectroscopy (PES) have been used. LEEM was first used to observe the surface morphologies of the prepared samples. In combination with LEEM instrument, low energy electron diffraction (LEED) was used to verify the existence of graphene on SiC substrate. The number of graphene layer was determined by collecting electron reflectivity at different electron energies. The number of dips observed in the electron reflectivity curve corresponds to the number of graphene layer. The experimental results obtained from LEEM and LEED have demonstrated that a film consisting of fairly large domains of 1 and 2 monolayer (ML) graphene was obtained by direct current heating of SiC under high vacuum (HV) condition with the based pressure of 10-6 Torr. A domain size in the range of up to about 5 to 10 μm have been observed. Meanwhile another graphene film prepared by the same method and the same temperature but under ultra high vacuum (UHV) condition with the based pressure of 10-10 Torr has much smaller domain size of 1 ML graphene compared to that grown under HV condition. We therefore suggested that the based pressure during the graphene growth has a strong influence on the morphology of graphene. This is because the Si evaporation rate is suppressed when heated in a high pressure environment, which normally leads to the improvement of the surface quality. The suppression of the Si evaporation rate has also been verified by a result obtained from the other sample directly heated under much higher based pressure, i.e. in an argon (Ar) environment of 1 atm. In addition to LEEM and LEED, the existence of graphene on SiC substrate has also been verified by the PES measurement. The C1s spectrum of graphene sample grown on SiC(0001) substrate showed three components, i.e. bulk SiC, graphene (G) and the buffer layer (B) located at 283.7 eV, 284.5 eV and 285.1 eV, respectively. The intensity ratios of the three components in the C1s spectrum were also used to estimate the number of graphene layer. The estimated number of graphene layer corresponds to the result obtained from LEEM.
2

Plasmonique, un outil pour l'ingénierie du champ électromagnétique aux petites échelles : Manipulation du champ proche optique / Plasmonics, a Tool for the Engineering of the Near Optical Field at the Nanometer Scale : Optical Near Field Manipulation

Mitiche, Sarra 25 September 2018 (has links)
À l'échelle nanométrique, les particules métalliques présentent de nouvelles propriétés optiques liées au phénomène de résonance plasmon de surface. Une résonance plasmon est une oscillation collective et cohérente des électrons de conduction à la surface d'une nanoparticule métallique sous l'influence d'un champ électromagnétique extérieur. La longueur d'onde de cette résonance ainsi que la distribution spatiale du champ électromagnétique associé dépendent des caractéristiques de la nanoparticule (taille, forme et nature chimique), du milieu diélectrique hôte et de la géométrie d'illumination. L’excitation de plasmons de surface génère des champs électromagnétiques locaux de fortes intensités, localisés en des points spécifiques de la nanoparticule, appelés «points chauds». La lumière est ainsi miniaturisée et confinée dans des espaces de taille sub-longueur d’onde (<20nm). La possibilité de produire et de contrôler ces points chauds augure d'importantes réalisations dans un large éventail de domaines d'applications allant des technologies de l'information aux énergies renouvelables, tout en passant par la biomédecine. Ce travail de thèse met en évidence la possibilité de générer et de manipuler des points chauds au niveau de structures de taille nanométrique par effet de la géométrie de la nanostructure métallique ou bien de la configuration et de la longueur d’onde de la lumière excitatrice. L’objectif est de manipuler la lumière à petite échelle afin de contribuer au développement de nouvelles technologies d’origine plasmonique. A cet égard, les réponses optiques de nano-objets métalliques de différentes géométries et tailles, pris individuellement : cube, prisme… ou en groupes: dimère, chaîne… sont étudiées par microscopie de photoémission d'électrons PEEM (PhotoEmission Electron Microscopy), une technique de cartographie haute résolution (20 nm), non intrusive, permettant un adressage sélectif des modes plasmons.Par ailleurs et également dans le cadre de ce travail, une méthode analytique de description du champ proche optique, basée sur la théorie des groupes, a été développée. Cette méthode permet de prédire et d’interpréter en quelques minutes le comportement plasmonique d’une particule à 2D ou 3D, de symétrie finie ou non, seules ou en dimères, à partir des symétries de l’objet et du champ excitateur. En complément, des simulations numériques par la méthode des éléments frontières BEM (Boundary Element Method) ont été effectuées. / At nanometer scale, the metallic particles exhibit new optical properties related to the surface plasmon resonance phenomenon. A plasmon resonance is a collective and coherent oscillation of the conduction electrons at a metallic nanoparticle surface under an external electromagnetic field. The resonance wavelength and the spatial distribution of the associated electromagnetic field depend on the nanoparticle characteristics (size, shape and chemical nature), the surrounding dielectric medium and the illumination geometry.The excitation of surface plasmons generates local electromagnetic fields of high intensity located at specific points of the nanoparticle called "hot spots". The light is miniaturized and confined in sub-wavelength areas (<20 nm). The ability to produce and control hot spots holds great promise for a large range of applications from information technology to renewable energies and biomedicine. This thesis highlights the possibility of generating and manipulating hot spots in nanostructures throughout the particle geometry or/and the configuration and wavelength of the exciting light. To do this, the optical response of various metallic nano-objects of different geometries and sizes, taken individually: cube, prism ... or in groups: dimer, chain ... are studied by PhotoEmission Electron Microscopy (PEEM), a non-intrusive and high resolution (20 nm) mapping technique allowing a selective addressing of plasmons modes. In addition to this experimental investigation, the search for a specific optical near-field distribution is also carried out using group theory. We developed an original theoretical method allowing to predict in a few minutes the plasmonic response of a 2D or 3D particle, of finite or infinite symmetry, alone or in dimer, from the object and exciting field symmetries. In parallel, numerical simulations using the Boundary Element Method (BEM) have been carried out.
3

Mécanismes de démouillage à l'état solide : Etude par microscopie à électrons lents des systèmes SOI et GOI / Mechanisms of solid-state dewetting

Passanante, Thibault 24 June 2014 (has links)
Ce travail de thèse est consacré à l’étude expérimentale des mécanismes de démouillage de films solides d’épaisseur nanométrique conduisant à la transformation d’un film mince en une assemblée d’îlots tridimensionnels. L’utilisation de la microscopie à électrons lents (LEEM) nous a permis d’étudier la morphologie et la cinétique in situ et en temps réel du démouillage de films de Si/SiO2 (SOI) et de Ge/SiO2 (GOI) obtenus par collage moléculaire (procédé Smart Cut™). Ces mesures expérimentales ont été complétées par des analyses par diffusion centrale des rayons X en incidence rasante (GISAXS) et des observations ex situ par microscopie à force atomique (AFM). Les mécanismes de démouillage de SOI et GOI sont thermodynamiquement pilotés par la capillarité et cinétiquement contrôlés par la diffusion de surface. L’étude complémentaire du démouillage à partir de fronts cristallographiquement orientés obtenus par lithographie nous a permis d’analyser le rôle central du facettage, de l’anisotropie cristalline et des processus de formation du bourrelet de démouillage. En particulier, le rôle de la nucléation 2D sur la cinétique d’épaississement (couche par couche) du bourrelet a pu être mis en évidence. Les résultats expérimentaux ont pu être confrontés à des modèles analytiques et des simulations de type Monte Carlo cinétique. Nous en avons déduit les valeurs des paramètres physiques pertinents et avons attribué les différences de morphologies entre SOI et GOI à la présence de facettes spécifiques. / This work is devoted to the experimental study of the dewetting mechanisms of ultrathin solid films by which a metastable film transforms into an assembly of tridimensional crystallites. Using low energy Electron Microscopy (LEEM) we analyse, in situ and in real time, the morphology and the kinetics of the dewetting of Si/SiO2 (SOI) and Ge/SiO2 (GOI) systems obtained by molecular bonding (Smart Cut™ process). Further information has been obtained by Grazing Incidence Small Angle X–ray Scattering (GISAXS) and Atomic Force Microscopy (AFM) measurements. We show that the dewetting is driven by surface free energy minimization and mediated by surface diffusion. A complementary study of artificial well-oriented dewetting fronts obtained by lithography enables us to analyze the important role played by facets, the crystal anisotropy and the rim thickening mechanism. We show that the rim thickening proceeds in a layer-by-layer mode and is limited by 2D nucleation. Thanks to analytical models and Kinetics Monte Carlo simulations, numerical values of the pertinent physical parameters involved in the dewetting process are obtained and the morphological differences between SOI and GOI are attributed to the presence of specific facets.
4

Topology of ferroelectric polarization at the BaTiO3(001) surface from ab initio calculations and electron microscopy-spectroscopy / Topologie de la polarisation ferroélectrique à la surface (001) de BaTiO3 par calculs ab initio et microscopie-spectroscopie d'électrons

Dionot, Jelle 15 September 2015 (has links)
À la surface ou à l’interface d’un matériau ferroélectrique, la polarisation peut être déstabilisée voire même annulée par le champ dépolarisation qui résulte de charges de polarisation non compensées. En l’absence de mécanismes d’écrantage extrinsèques (adsorbats, électrodes) ou intrinsèques (défauts, dopants), l’ordonnancement en domaines est le moyen le plus naturel dont un système a recourt pour rester ferroélectrique et minimiser son énergie électrostatique. Cette thèse se concentre sur l’étude de la stabilité de multiples configurations en domaines, ainsi que de la façon dont elle dépend de facteurs géométriques, chimiques et élastiques, à la surface du BaTiO3(001).Des calculs ab initio, fondés sur la théorie de la fonctionnelle de la densité, ont été menés pour éclaircir l’influence de la terminaison de surface, de la contrainte parallèle à la surface, de l’épaisseur du système et de la taille des domaines sur la polarisation de différentes phases ferroélectriques dans des couches ultraminces. L’effet de lacunes d’oxygène en surface sur la polarisation et sur la structure électronique a aussi été étudié. La microscopie d’électrons lents (LEEM) et la microscopie d’électrons photoémis (PEEM) ont été utilisées pour étudier les propriétés de la polarisation à la surface de monocristaux de BaTiO3 réduit, afin d’examiner l’influence des lacunes d’oxygène sur la polarisation ferroélectrique par une approche expérimentale, renforçant ainsi les résultats de calculs. / At a surface or interface of a ferroelectric material, the polarization can be destabilized and even suppressed by the depolarizing field which arises from uncompensated polarization charge. In the absence of external (adsorbates, electrodes) or internal (defects, dopants) screening mechanisms, domain ordering is the most natural way for a system to remain ferroelectric and minimize its electrostatic energy. This thesis focuses on the study of the stability of various possible domain configurations, and on how it depends and interplays on size, chemical and elastic factors, at the (001) surface of BaTiO3.First-principles calculations, based on density functional theory, have been performed to enlighten the influence of surface terminations, in-plane strain, system thickness and domain size in ultrathin films on the polarization in different ferroelectric phases. The effect of surface oxygen vacancies on the polarization and electronic structure has also been investigated. Low Energy electron microscopy (LEEM) and photoemission electron microscopy (PEEM) have been used to study the surface properties of ferroelectric polarization in reduced BaTiO3 single crystals, allowing to address the influence of oxygen vacancies on the ferroelectric polarization from experimental approaches, supporting the calculations results.
5

Surface stress and large-scale self-organization at organic-metal interfaces / Oberflächenspannung und langreichweitige Selbstorganisation an Organik-Metall Grenzflächen

Pollinger, Florian January 2008 (has links) (PDF)
Anhand von Modellsystemen wurde in dieser Arbeit die Bedeutung elastischer Wechselwirkungen an Organik-Metall Grenzflächen, insbesondere für die Selbstorganisierte Ausbildung periodisch facettierter Strukturen, untersucht. Die Änderung der Oberflächenspannung während der Ausbildung der Grenzfläche zwischen 3,4,9,10-Perylentetracarbonsäuredianhydrid (PTCDA) und Ag(111) wurde mit der Biegekristalltechnik gemessen. Es ist bekannt, dass dieses System durch eine chemisorptive Bindung bestimmt wird. In der Tat stimmen Vorzeichen und Bedeckungsabhängigkeit mit Vorhersagen und Experimenten aus der Literatur zu chemisorptiv bestimmten Grenzflächen überein. Während der Einbau von Molekülen in große Domänen die Oberflächenspannung verringert, führt das Auftreten von fehlerhaften Domänengrenzen zu einer Erhöhung der Oberflächenspannung. Die absolute Änderung der Oberflächenspannung in der Höhe von (0.30 +- 0.10) N/m ist in der relativ schwachen Wechselwirkung des PTCDA Moleküls mit einem einzelnen Silberatom begründet. Es soll jedoch betont werden, dass dieser Wert einer Oberflächenspannungsänderung von (2.2 +- 0.2) eV pro Molekül entspricht, die damit in derselben Größenordnung wie die vermutete Bindungsenergie des Systems liegt. Daher zeigen diese Experimente, dass elastische Wechselwirkungen eine nicht zu vernachlässigende Rolle in dieser ganzen Materialklasse spielen können. Dadurch tragen die Experimente eine neue Sichtweise zum Verständnis dieser Grenzflächen bei. Ferner etablieren sie die Biegekristalltechnik auf dem ganzen Feld der Organik-Metall Grenzflächen, da die Ergebnisse in Einklang mit den wohlbekannten Eigenschaften des Systems liegen. Schon der Nachweis einer Durchbiegung der Probe ist speziell für die Grenzfläche PTCDA/Ag(111) von Bedeutung. Dieser Effekt ist der erste experimentelle Nachweis einer strukturellen Änderung in den obersten Substratatomlagen während der Adsorption von PTCDA auf Ag(111). Da eine solche Modifikation nicht zu vernachlässigende Konsequenzen für die Interpretation anderer experimenteller Ergebnisse hat, erscheinen weitere Studien mit anderen, quantitativeren strukturellen Methoden notwendig. Der Schwerpunkt dieser Arbeit lag jedoch auf der Untersuchung der Ausbildung der langreichweitigen, selbstorganisierten Ordnung der facettierten PTCDA/Ag(10 8 7) Grenzfläche. Der reziproke Raum dieser Grenzfläche wurde sowohl mit mittelnder hochauflösender Elektronenbeugung (SPA-LEED) als auch mit lokaler Elektronenbeugung in der Mikroskopie niederenergetischer Elektronen (LEEM) kartiert. Außerdem wurden diese reziproken Daten durch mikroskopische LEEM Realraumdaten komplementär ergänzt um die Morphologie der Grenzfläche zu charakterisieren. Für die gewählte Präparationsart, Adsorption der Moleküle auf das 550 K warme Substrat, wurden sechs verschiedene Facettentypen ((111), (532), (743),(954), (13 9 5) und (542)) beobachtet. Diese Facettentypen treten in homogenen, mikrometergroßen Gebieten auf der Oberfläche auf, wie Dunkelfeld-LEEM Aufnahmen zeigen. Wenn jedoch die ursprüngliche mesoskopische Orientierung der Oberfläche lokal von der Durchschnittsorientierung z.B. in Bezug auf die ursprüngliche Stufendichte abweicht, werden an dieser Stelle andere Facettentypen gebildet und damit das ansonsten regelmäßige Muster gestört. Sowohl der Grad der erreichten Ordnung der facettierten Grenzfläche als auch die gebildeten Facettentypen hängen somit stark von der ursprünglichen mesoskopischen Morphologie des sauberen Substrates ab. Um das Verständnis der kinetischen Prozesse zu verbessern wurde die Temperaturabhängigkeit der Ausbildung der Grenzfläche in einem Temperaturbereich zwischen 418 K und 612 K untersucht. Bei niedrigen Wachstumstemperaturen traten zusätzliche, steilere Facetten mit einem Neigungswinkel von 27° gegenüber der (111) Fläche auf. Weiterhin wurde mit facetten-sensitivem Dunkelfeld-LEEM die Größen- sowie die räumliche Verteilung ausgewählter Facettentypen bei den verschiedenen Temperaturen untersucht. Die Nukleationsdichte der Facetten zeigte dabei keine Temperaturabhängigkeit. Eine Diffusionslimitierung der Nukleation kann daher ausgeschlossen werden. Darüber hinaus wurden die Ausmaße der Facetten statistisch ausgewertet. Die absolute Facettengröße folgt einer exponentiellen Verteilung, was auf ein zufallsgetriebenes Wachstum und das Fehlen einer Wechselwirkung der Facetten untereinander hinweist. Während die Facettenlängen ebenso einer exponentiellen Verteilung unterliegen, ist die Breitenverteilung durch ein Maximum ausgezeichnet. Letztere Verteilung spiegelt den hohen Grad an lateraler Ordnung in dem System wieder. Diese Anisotropie hängt von der Temperatur ab und kann bei Substrattemperaturen über 478 K während des Wachstums beobachtet werden. Die Existenz eines Maximums in einer solchen Größenverteilung weist auf eine langreichweitige Wechselwirkung hin, die die strukturelle Ordnung induziert. Die Natur dieser langreichweitigen Wechselwirkung wurde mit drei komplementären in-situ Methoden untersucht, wobei jeweils neue Einblicke in die Ausbildung von facettierten Organik-Metall-Grenzflächen gewonnen werden konnten: Die Biegekristalltechnik, hochauflösende Beugung niederenergetischer Elektronen (SPALEED), sowie deren Mikroskopie (LEEM). Die Biegekristalltechnik wurde das erste Mal überhaupt auf ein facettierendes System angewendet. Unterhalb der kritischen Temperatur des Facettierungsüberganges ähnelt die Oberflächenspannungsänderung während der Bildung der PTCDA/Ag(10 8 7)-Grenzflächenbildung sowohl in funktionaler Abhängigkeit als auch in der Größenordnung der für die Referenzgrenzfläche PTCDA/Ag(111) beobachteten. Oberhalb der Übergangstemperatur beobachtet man jedoch für die ausfacettierte PTCDA/Ag(10 8 7) Grenzfläche mit (0.67 +- 0.10) N/m eine bedeutend größere Oberflächenspannungsänderung als in den vorherigen Fällen. Zudem ändert sich die Oberflächenspannung in klar unterscheidbaren Schritten mit einer eindeutig auflösbaren Feinstruktur aus positiven und negativen Spannungsänderungen. Diese einzelnen Phasen in der Änderung der Oberflächenspannung können Stufen in der Entwicklung der Strukturüberganges dieses Systems zugeordnet werden, die mit den strukturellen Charakterisierungsmethoden beobachtet wurden. Durch diese Identifikation werden morphologischen Objekten, also den Facetten, ein eigener besonderer Spannungscharakter zugeordnet. Somit werden aber auch Spannungsdomänen auf der Oberfläche identifiziert. Die Existenz dieser Spannungsdomänen ist nun aber die Vorraussetzung für die Anwendung von elastizitätsbasierten Kontinuumsbeschreibungen des Selbstordnungseffektes. Daher stellen diese Ergebnisse den ersten experimentellen Nachweis dar, dass diese Kontinuumsbeschreibungen der Selbstorganisation tatsächlich auch auf die gesamte Materialklasse der facettierenden Organik-Metall-Grenzflächen angewendet werden können. Zusammengefasst sind diese Ergebnisse starke Beweise dafür, dass elastische Wechselwirkungen der physikalische Ursprung der langreichweitigen Ordnung dieses Systems sind. Weiterhin legt die eindeutige Korrelation zwischen strukturellem Phasenübergang und Oberflächenspannungsänderung auch nahe, dass letzterer ebenso eine wichtige Rolle in der Kinetik des Systems spielt. Tatsächlich scheint das System zu versuchen die Gesamtänderung der Oberflächenspannung während der Grenzflächenbildung durch die Bildung von Facettentypen positiven und negativen Charakters zu begrenzen. Daher könnte die Art ihres Beitrags zur Oberflächenspannungsänderung darüber entscheiden, ob eine bestimmte Facettenorientierung gebildet wird oder nicht. Auch scheint das System sich bei hohen Bedeckungen unter anderem deshalb erneut umzufacettieren um der Bildung von fehlerhaften Domänengrenzen entgegenzuwirken, die mit einem Anstieg der Oberflächenspannung verbunden wären. Schließlich wurde im Rahmen dieser Arbeit noch das templatunterstützte Wachstum lateraler, heteroorganischer Nanostrukturen untersucht. Dabei wurde ein zweites, typisches molekulares Modellsystem, sogenannte "Selbstassemblierte Monolagen", auf der teilbedeckten PTCDA/Ag(10 8 7) Grenzfläche aufgewachsen. Mit Standardmethoden der Oberflächencharakterisierung konnte nachgewiesen werden, dass die grundlegenden Eigenschaften dieses Wachstumsprinzips im Experiment in der Tat erreicht werden. / The role of elastic interactions, particularly for the self-organized formation of periodically faceted interfaces, was investigated in this thesis for archetype organic-metal interfaces. The cantilever bending technique was applied to study the change of surface stress upon formation of the interface between 3,4,9,10-perylene-tetracarboxylic-dianhydride (PTCDA) and Ag(111). This system is known to form a chemisorptive bonding. Indeed, the sign and the coverage-dependence of the surface stress change are in agreement to models and previous measurements of chemisorptive systems in literature. While the adsorption of molecules into the large domains is associated with a negative, i.e. compressive stress change, the formation of domain boundaries in the molecular layer induces a stress change of opposite sign, increasing the surface stress. The magnitude of the surface stress change of (-0.30 +- 0.10} N/m reflects a relatively weak binding of a PTCDA molecule to each individual single silver atom. It is emphasized, however, that if normalized to the surface stress change per molecule, this value corresponds to a stress change of (-2.2 +- 0.2) eV per molecule which is in the order of the suspected binding energy of this system. Therefore, these experiments reveal elastic interactions to be of significant order of magnitude for this system class. Thereby, they add a new point of view to the understanding of these interfaces. Besides, since the results are in agreement with the well-known properties of this interface, they establish the cantilever bending technique in the field of organic-metal interfaces. The mere existence of a bending of the sample implies an interesting detail for the PTCDA/Ag(111) interface in particular. It is the first experimental evidence for a structural change in the topmost substrate layers upon adsorption of PTCDA on Ag(111). Since such a modification has significant implications for the interpretation of other experimental results, a further investigation with more quantitative structural methods appears necessary. The main focus of this work, however, was on the investigation of the formation of the long-range ordered, self-organized faceted PTCDA/Ag(10 8 7) interface. Reciprocal space maps of this interface were recorded both by spot profile analysis low energy electron diffraction (SPA-LEED) and low energy electron microscopy (LEEM) in selected area LEED mode. Complementary to the reciprocal data, also microscopic real-space LEEM data were used to characterize the morphology of this interface. Six different facet faces ((111), (532), (743), (954), (13 9 5), and (542)) were observed for the preparation path of molecular adsorption on the substrate kept at 550 K. Facet-sensitive dark-field LEEM localized these facets to grow in homogeneous areas of microscopic extensions. If the pristine mesoscopic orientation locally deviates from the average orientation, e.g. in pristine step density, locally different facet types are formed, distorting the otherwise regular mesoscopic pattern. Hence, the original mesoscopic orientation of the substrate strongly determines the degree of order of the faceted surface and the facet species formed. The temperature-dependence of the interface formation was studied in a range between 418 K and 612 K in order to learn more about the kinetics of the process. Additional steeper facets of 27° inclination with respect to the (111) surface were observed in the low temperature regime. Furthermore, using facet-sensitive dark-field LEEM, spatial and size distributions of specific facets were studied for the different temperatures. The nucleation density of the facets did not depend on temperature and can therefore be concluded not to be limited by diffusion. Moreover, the facet dimensions were statistically analyzed. The total island size of the facets follows an exponential distribution, indicating a random growth mode in absence of any mutual facet interactions. While the length distribution of the facets also follows an exponential distribution, the width distribution is peaked, reflecting the high degree of lateral order. This anisotropy is temperature-dependent and occurs starting above 478 K substrate temperature during growth. The peaked distribution indicates the presence of a long-range interaction which leads to the structural order of the self-organized grating. The origin of this long-range interaction was investigated combining three complementary in-situ methods, all providing new insights into the formation of faceted organic-metal interfaces: the cantilever bending technique, high-resolution low energy electron diffraction (SPA-LEED), and microscopy (LEEM). The cantilever bending technique was applied for the first time to a faceting system at all. Below the faceting transition temperature the surface stress change associated with the formation of the PTCDA/Ag(10 8 7) interface resembles in shape and magnitude the one observed for the reference interface PTCDA/Ag(111). But above the transition temperature the absolute surface stress change of (-0.67 +- 0.10) N/m observed for the faceted PTCDA/Ag(10 8 7) interface is considerably larger than for the previous cases. Moreover, the stress change happens in distinguishable stages with a clearly resolvable fine structure of regimes of positive and negative stress changes. These different regimes of surface stress change can be correlated to different stages of the structural phase transition observed by the structural in-situ methods. Thereby, morphological objects (i.e. the facets) are assigned to a specific stress character. Thus, domains of different stress character can be identified on the surface. These stress domains are the prerequisite to apply continuum descriptions of the self-ordering process based on elastic interactions. Hence, the results are the first experimental verification that these continuum descriptions are indeed also applicable to the whole system class of faceting organic-metal interfaces. In conclusion, the results provide strong evidence for elastic interactions being the physical origin of long-range order for this system. In addition, the clear correlation of structural phase transition and surface stress change regimes suggests surface stress to play also an important role for the kinetics of the system. Indeed, the system seems to try to limit the overall stress change during the interface formation by forming facets of positive and negative stress character. Hence, the selection of specific facets could depend on the corresponding stress character. Furthermore, the system seems willing to re-facet at high coverages in order to prevent imperfect domain boundaries which are associated with an increase of surface stress. Finally, template-assisted growth of lateral, heterorganic nanostructures has been explored. Therefore, self-assembled monolayers as a second archetype class of molecules were grown on partially covered PTCDA/Ag(10 8 7) interfaces. Indeed, using standard surface science techniques, the basic principle of this growth scheme was confirmed to be successful.
6

Controlling Electronic and Geometrical Structure of Honeycomb-Lattice Materials Supported on Metal Substrates : Graphene and Hexagonal Boron Nitride

Vinogradov, Nikolay January 2013 (has links)
The present thesis is focused on various methods of controlling electronic and geometrical structure of two-dimensional overlayers adsorbed on metal surfaces exemplified by graphene and hexagonal boron nitride (h-BN) grown on transition metal (TM) substrates. Combining synchrotron-radiation-based spectroscopic and various microscopic techniques with in situ sample preparation, we are able to trace the evolution of overlayer electronic and geometrical properties in overlayer/substrate systems, as well as changes of interfacial interaction in the latter.It is shown that hydrogen uptake by graphene/TM substrate strongly depends on the interfacial interaction between substrate and graphene, and on the geometrical structure of graphene. An energy gap opening in the electronic structure of graphene on TM substrates upon patterned adsorption of atomic species is demonstrated for the case of atomic oxygen adsorption on graphene/TM’s (≥0.35 eV for graphene/Ir(111)). A non-uniform character of adsorption in this case – patterned adsorption of atomic oxygen on graphene/Ir(111) due to the graphene height modulation is verified. A moderate oxidation of graphene/Ir(111) is found largely reversible. Contrary, oxidation of h-BN/Ir(111) results in replacing nitrogen atoms in the h-BN lattice with oxygen and irreversible formation of the B2O3 oxide-like structure.      Pronounced hole doping (p-doping) of graphene upon intercalation with active agents – halogens or halides – is demonstrated, the level of the doping is dependent on the agent electronegativity. Hole concentration in graphene on Ir(111) intercalated with Cl and Br/AlBr3 is as high as ~2×1013 cm-2 and ~9×1012 cm-2, respectively.     Unusual periodic wavy structures are reported for h-BN and graphene grown on Fe(110) surface. The h-BN monolayer on Fe(110) is periodically corrugated in a wavy fashion with an astonishing degree of long-range order, periodicity of 2.6 nm, and the corrugation amplitude of ~0.8 Å. The wavy pattern results from a strong chemical bonding between h-BN and Fe in combination with a lattice mismatch in either [11 ̅1] or [111 ̅] direction of the Fe(110) surface. Two primary orientations of h-BN on Fe(110) can be observed corresponding to the possible directions of lattice match between h-BN and Fe(110).     Chemical vapor deposition (CVD) formation of graphene on iron is a formidable task because of high carbon solubility in iron and pronounced reactivity of the latter, favoring iron carbide formation. However, growth of graphene on epitaxial iron films can be realized by CVD at relatively low temperatures, and the formation of carbides can be avoided in excess of the carbon-containing precursors. The resulting graphene monolayer creates a periodically corrugated pattern on Fe(110): it is modulated in one dimension forming long waves with a period of ~4 nm parallel to the [001] direction of the substrate, with an additional height modulation along the wave crests. The novel 1D templates based on h-BN and graphene adsorbed on iron can possibly find an application in 1D nanopatterning. The possibility for growing high-quality graphene on iron substrate can be useful for the low-cost industrial-scale graphene production.
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Samouspořádané molekulární vrstvy na povrchu epitaxního grafenu / Self-assembled molecular layers on epitaxial graphene

Kovařík, Štěpán January 2018 (has links)
Samouspořádání organických molekul je spontánní proces tvorby nanostruktur, při kterém je výsledná struktura určena mezimolekulárními and molekulárně-substrátovými interakcemi. Pochopení principů samouspořádávání je klíčem k přípravě funkčních nanostruktur s atomární přesností. Tato diplomová práce se zaměřuje na přípravu a studium samouspořádaných molekulárních struktur 4,4’-diphenyl dikarboxylové kyseliny na povrchu grafenu připraveného na Ir(111). Pro studium vlastností molekulárních struktur je využito rastrovací tunelovací mikroskopie a nízkoenergiové elektronové mikroskopie. Tato kombinace umožňuje získat informace z oblastí o velikosti v řádu nanometrů až milimetrů. V práci je popsána molekulární strukuktura stabilní při pokojové teplotě. Vazebný motiv této struktury je dán interakcí karboxylových skupin sousedních molekul.
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Kalibrace a interpretace obrazových dat měřených zařízením LEEM / Calibration and interpretation of images measured by LEEM

Endstrasser, Zdeněk January 2021 (has links)
This thesis deals with the software development to calibration and interpretation of image data measured by a LEEM device. As the imaging technique is uniquely suited for in-situ studies of surface dynamical processes, the attention is mainly paid to methods enabling the evaluation of measurement time series. The phase correlation method based on Fourier transform of images is proposed to temperature shift correction between consecutive frames. The thesis describes the methods of additive and impulse noise filtering, image visualization, the filtration of secondary electrons and the determination of I-V curves from measured image data. Implemented methods are described not only in terms of their mathematical origin, but also with emphasis on the revealing of critical aspects associated with their use. The thesis also focuses on the application of the created algorithm to image data capturing the spatial and temporal evolution of 4,4’-biphenyl-dicarboxylic acid surface phases induced by sample annealing. Based on these evaluations, a suitable procedure is then determined to perform accurate detection and compensation of temperature shift said.
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Zpracování signálů z moderních mikroskopů pro lokální charakterizaci materiálů / Processing of modern microscope signals for local material characterization

Kaspar, Pavel January 2013 (has links)
Signal processing from modern microscopes for local characteristics of materials Image processing is more and more important for the advancement of image evaluation taken from microscopes. This thesis engages the problem of artefact detection and removal from images taken by electron microscope, more accurately by low energy electron microscopy (LEEM). It then offers a possible course of processing such images by edge detection and its theoretical use. These operations are all made in MatLAB language.
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Tailoring nanoscale metallic heterostructures with novel quantum properties

Sanders, Charlotte E. 2013 May 1900 (has links)
Silver (Ag) is an ideal low-loss platform for plasmonic applications, but from a materials standpoint it presents challenges. Development of plasmonic devices based on Ag thin film has been hindered both by the dificulty of fabricating such film and by its fragility out of vacuum. Silver is non-wetting on semiconducting and insulating substrates, but on certain semiconductors and insulators can adopt a metastable atomically at epitaxial film morphology if it is deposited using the "two-step" growth method. This method consists of deposition at low temperature and annealing to room temperature. However, epitaxial Ag is metastable, and dewets out of vacuum. The mechanisms of dewetting in this system remain little understood. The fragility of Ag film presents a particular problem for the engineering of plasmonic devices, which are predicted to have important industrial applications if robust low-loss platforms can be developed. This dissertation presents two sets of experiments. In the first set, scanning probe techniques and low energy electron microscopy have been used to characterize Ag(111) growth and dewetting on two orientations of silicon (Si), Si(111) and Si(100). These studies reveal that multiple mechanisms contribute to Ag film dewetting. Film stability is observed to increase with thickness, and thickness to play a decisive role in determining dewetting processes. A method has been developed to cap Ag film with germanium (Ge) to stabilize it against dewetting. The second set of experiments consists of optical studies that focus on the plasmonic properties of epitaxial Ag film. Because of the problems posed until now by epitaxial Ag growth and stabilization, research and development in the area of plasmonics has been limited to devices based on rough, thermally evaporated Ag film, which is robust and simple to produce. However, plasmonic damping in such film is higher than in epitaxial film. The optical studies presented here establish that Ag film can now be stabilized sufficiently to allow optical probing and device applications out of vacuum. Furthermore, they demonstrate the superiority of epitaxial Ag film relative to thermally evaporated film as a low-loss platform for plasmonic devices spanning the visible and infrared regimes. / text

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