This thesis presents several experiments, generally aiming at visualising the ballistic and topological transport on the high-mobility graphene/boron nitride heterostructure using the scanning gate microscope. For the first experiment, we use the scanning gate microscopy to map out the trajectories of ballistic carriers in high-mobility graphene encapsulated by hexagonal boron nitride and in a weak perpendicular magnetic field. We employ a magnetic focusing transport configuration to image carriers that emerge ballistically from an injector, follow a cyclotron path due to the Lorentz force from an applied magnetic field, and land on an adjacent collector probe. The local potential generated by the scanning tip in the vicinity of the carriers deflects their trajectories, modifying the proportion of carriers focused into the collector. By measuring the voltage at the collector while scanning the tip, we are able to obtain images with arcs that are consistent with the expected cyclotron motion. We also demonstrate that the tip can be used to redirect misaligned carriers back to the collector. For the second experiment, we investigate the graphene van der Waals structures formed by aligning monolayer graphene with insulating layers of hexagonal boron nitride which exhibit a moiré superlattice that is expected to break sublattice symmetry. However, despite an energy gap of several tens of millielectronvolts opening in the Dirac spectrum, electrical resistivity remains lower than expected at low temperature and varies between devices. While subgap states are likely to play a role in this behaviour, their precise nature is still unclear in the community. We therefore perform a scanning gate microscopy study of graphene moiré superlattice devices with comparable activation energy but with different charge disorder levels. In the device with higher charge impurity ($\sim$ 10$^-$ cm$^{-2}$) and lower resistivity ($\sim$ 10 k$\Omega$) at the Dirac point we observe scanning gate response along the graphene edges. Combined with simulations, our measurements suggest that enhanced edge doping is responsible for this effect. In addition, a device with low charge impurity ($\sim$ 10$^{9}$ cm$^{-2}$) and higher resistivity ($\sim$ 100 k$\Omega$) shows subgap states in the bulk. Our measurements provide alternative model to the prevailing theory in the literature in which the topological bandstructures of the graphene moiré superlattices entail an edge currents shunting the insulating bulk. In the third experiment, we continue our study in the graphene moir$\acute e$ superlattices with the newly reported non-local Hall signals at the main Dirac point. It has been associated with the non-zero valley Berry curvature due to the gap opening and the nonlocal signal has been interpreted as the signature of the topological valley Hall effects. However, the nature of such signal is still disputed in the community, due to the vanishing density of states near the Dirac point and the possible topological edge transport in the system. Various artificial contribution without a topological origin of the measurement scheme has also been suggested. In connection to the second experiment, we use the scanning gate microscope to image the non-local Hall resistance as well as the local resistance in the current path. By analysing the features in the two sets of images, we find evidence for topological Hall current in the bulk despite a large artificial components which cannot be distinguished in global transport measurement. In the last experiment, we show the development of a radio-frequency scanning impedance microscopy compatible with the existing scanning gate microscopy and the dilution refrigerator. We detailed the design and the implementation of the radio-frequency reflectometry and the specialised tip holder for the integration of the tip and the transmission lines. We demonstrate the capability of imaging local impedance of the sample by detecting the mechanical oscillation of the tip, the device topography, and the Landau levels in the quantum Hall regime at liquid helium temperature and milli-Kelvin temperature.

The work of this thesis comprises extensive Noncontact Atomic Force Microscopy (NC-AFM) characterization of clean metal-oxide (YSZ(100)/(111) and MgO(100)) and graphitic (HOPG) supports as templates for the novel, photochemically induced nucleation of cobalt oxide nanostructures, particularly Cobalt (III) Oxide. The nanostructure-support surfaces were also studied by X-ray Photoelectron Spectroscopy (XPS) to verify the nature of the supported cobalt oxide and to corroborate the surface topographic and phase NC-AFM data. Heteroepitaxial growth of Co2O3 nanostructures proves to exhibit a variety of different growth modes based on the structure of the support surface. On this basis, single-crystal support surfaces ranging from nonpolar to polar and atomically flat to highly defective and reactive were chosen, again, yielding numerous substrate-nanostructure interactions that could be probed by high-performance surface science techniques.

This thesis examines and exploits the optical properties of pairs of MNPs. Pairs of MNPs offer two further parameters not existent at single MNPs, which both affect the local optical fields in their vicinity: the distance between them, and their relative orientation with respect to the polarisation of the excitation light. These properties are subject of three chapters: One section examines the distance-dependent and orientation-sensitive scattering cross section (SCS) of two equally sized MNPs. Both near- and far-field interactions affect the spectral position and spectral width of the SCS. Far-field coupling affects the SCS even in such a way that a two-particle system may show both a blue- and redshifted SCS, depending only on the distance between the two MNPs. The maximum distance for this effect is the coherence length of the illumination source – a fact of importance for SCS-based experiments using laser sources. Another part of this thesis examines the near-field between two MNPs and the dependence of the locally enhanced field on the relative particle orientation with respect to the polarisation of the excitation light. To attain a figure of merit, the intensity of fluorescence light from dye molecules in the surrounding medium was measured at various directions of polarisation. The field enhancement was turned into fluorescence enhancement, even providing a means for sensing the presence of very small MNPs of 12 nm in diameter. In order to quantify the near-field experimentally, a different technique is devised in a third section of this thesis – scanning particle-enhanced Raman microscopy (SPRM). This device comprises a scanning probe carrying an MNP which in turn is coated with a molecule of known Raman signature. By manoeuvring this outfit MNP into the vicinity of an illuminated second MNP and by measuring the Raman signal intensity, a spatial mapping of the field enhancement was possible. / Diese Dissertation untersucht und nutzt die optischen Eigenschaften von Paaren von Metall-Nanopartikeln (MNP). MNP-Paare bieten gegenüber einzelnen MNP zwei weitere Parameter, welche beide auf das optische Nahfeld der zwei MNPs wirken: zum Einen der Abstand der zwei MNPs zueinander, zum Anderen die relative Ausrichtung des Paares bezüglich der Polarisation des anregenden Lichts. Diese Eigenschaften sind Thema der Arbeit: Ein Abschnitt untersucht den abstands- und orientierungsabhängigen Streuquerschnitt (SQS) zweier gleichgroßer MNPs. Die spektrale Position und die Breite des SQS wird von Wechselwirkungen sowohl im Nah- als auch im Fernfeld beeinflusst. Der Einfluß der Fernfeld-Wechselwirkung geht so weit, daß ein Zwei-MNP-System sowohl einen blau- als auch einen rotverschobenen SQS haben kann – dies hängt lediglich vom Abstand der zwei MNPs ab. Die Reichweite dieser Fernfeld-Wechselwirkung wird durch die Kohärenzlänge der Beleuchtungsquelle bestimmt – eine wichtige Tatsache für SQS-Untersuchungen, welche Laserquellen verwenden. Ein weiterer Teil der Dissertation untersucht das Nahfeld zwischen zwei MNPs. Insbesondere wird dargestellt, inwieweit die Überhöhung des Nahfelds von der Orientierung des Partikelpaares bezüglich der Polarisation des Anregungslichts abhängt. Um den Effekt quantifizieren zu können, wurde die Intensität der Fluoreszenz des umgebenden Mediums für verschiedene Polarisationsrichtungen gemessen. Die lokale Feldverstärkung konnte in eine Fluoreszenzverstärkung gewandelt werden, mit deren Hilfe sich sogar die Anwesenheit sehr kleiner MNPs von nur 12 nm Durchmesser nachweisen ließ. Wie Nahfeld-Intensitäten experimentell quantifiziert werden können, stellt ein dritter Abschnitt dieser Dissertation vor – per MNP-verstärkter Raman-Rastersonden-Mikroskopie. Diese Technik besteht aus einer Rastersonde, welcher ein MNP anheftet, welches wiederum mit einem Molekül bekannter Ramansignatur überzogen ist. Indem solch eine Sonde in die unmittelbare Nähe eines zweiten, beleuchteten MNPs gebracht wurde und dabei die Intensität des Raman-Signals aufgezeichnet wurde, ließ sich die räumliche Verteilung der Ramanverstärkung vermessen.

Modification of the properties of solid state structures, used for gas sensing is important task in making detection and measurement systems of volatile chemical compounds. These properties depend on material, inner structure and interaction with gas atmosphere. In hybrid materials (solid-biomolecular) biochemical recognition plays important role in gas sensing mechanism. In this work the methodologies of the SPM was applied for characterization of the local point and local area properties in the gas sensitive MO films with the nanoscaled thickness that can be used for nanosystems and hybrid materials in novel types of chemical detectors. In this dissertation morphology and physical properties of metal oxide films with thickness from a few to about 50 nm was investigated and described a relationship between the gas response and film thickness. It was experimentally shown that effects of external influence on the properties of the surface nanostructures can be described by the specific characteristics of the scanning probe spectroscopy displaying the dependences of the probe contact electric current on both the probe potential and the probe pressing force. An original method based on the SPM probe controlled electrical current was proposed for the formation of nanosystems with various electrical properties on the surfaces of thin MO films. / Kryptingas kietojo kūno darinių, naudojamų išorinio dujų poveikio detekcijai, savybių keitimas yra vienas iš aktualiausių uždavinių, sprendžiamų kuriant lakiųjų cheminių junginių poveikio atpažinimo ir matavimo sistemas. Šias savybes lemia darinių medžiaga, jų struktūra bei sąveikos su dujine aplinka ypatumai, kurie hibridiniuose dariniuose iš kietojo kūno ir biomolekulių gali būti lemiami dar ir biocheminiu atpažinimu. Šiame darbe tiriami dujoms jautrūs hibridiniai dariniai ir nanosistemos, integruotos metalo oksido plėvelėse, Skenuojančio zondo mikroskopijos (SZM) metodais. Disertacijoje susieti itin plonų (<30-50 nm) SnOx sluoksnių varžos atsako į dujas bei elektrinių savybių ypatumai su sluoksnių morfologija, priklausančia nuo auginimo sąlygų ir trukmės. Eksperimentiškai įrodyta, jog SZM lokalinių srovių tyrimai, priklausomai nuo matavimo parametrų, leidžia atskirai aprašyti technologiškai keičiamas dujoms jautrių darinių charakteristikas ir tik nanosistemose vykstančius procesus, kurie, kai kuriais atvejais, gali būti stebimi ir tipiškuose dujoms jautrių darinių taikymuose. Sukurtas originalus metodas, tinkantis nanostruktūroms metalo oksidų paviršiuje formuoti bei tų struktūrų elektrinėms savybėms keisti. Skirtingai nuo literatūroje žinomo paviršiaus nanooksidinimo, pritaikyto formuoti cheminiam poveikiui atsparias dangas, mūsų metodas leidžia formuoti įvairaus elektrinio laidumo nanostruktūras metalo oksidų paviršiuje.

Kryptingas kietojo kūno darinių, naudojamų išorinio dujų poveikio detekcijai, savybių keitimas yra vienas iš aktualiausių uždavinių, sprendžiamų kuriant lakiųjų cheminių junginių poveikio atpažinimo ir matavimo sistemas. Šias savybes lemia darinių medžiaga, jų struktūra bei sąveikos su dujine aplinka ypatumai, kurie hibridiniuose dariniuose iš kietojo kūno ir biomolekulių gali būti lemiami dar ir biocheminiu atpažinimu. Šiame darbe tiriami dujoms jautrūs hibridiniai dariniai ir nanosistemos, integruotos metalo oksido plėvelėse, Skenuojančio zondo mikroskopijos (SZM) metodais. Disertacijoje susieti itin plonų (< 30-50 nm) SnOx sluoksnių varžos atsako į dujas bei elektrinių savybių ypatumai su sluoksnių morfologija, priklausančia nuo auginimo sąlygų ir trukmės. Eksperimentiškai įrodyta, jog SZM lokalinių srovių tyrimai, priklausomai nuo matavimo parametrų, leidžia atskirai aprašyti technologiškai keičiamas dujoms jautrių darinių charakteristikas ir tik nanosistemose vykstančius procesus, kurie, kai kuriais atvejais, gali būti stebimi ir tipiškuose dujoms jautrių darinių taikymuose. Sukurtas originalus metodas, tinkantis nanostruktūroms metalo oksidų paviršiuje formuoti bei tų struktūrų elektrinėms savybėms keisti. Skirtingai nuo literatūroje žinomo paviršiaus nanooksidinimo, pritaikyto formuoti cheminiam poveikiui atsparias dangas, mūsų metodas leidžia formuoti įvairaus elektrinio laidumo nanostruktūras metalo oksidų paviršiuje. / Modification of the properties of solid state structures, used for gas sensing is important task in making detection and measurement systems of volatile chemical compounds. These properties depend on material, inner structure and interaction with gas atmosphere. In hybrid materials (solid-biomolecular) biochemical recognition plays important role in gas sensing mechanism. In this work the methodologies of the SPM was applied for characterization of the local point and local area properties in the gas sensitive MO films with the nanoscaled thickness that can be used for nanosystems and hybrid materials in novel types of chemical detectors. In this dissertation morphology and physical properties of metal oxide films with thickness from a few to about 50 nm was investigated and described a relationship between the gas response and film thickness. It was experimentally shown that effects of external influence on the properties of the surface nanostructures can be described by the specific characteristics of the scanning probe spectroscopy displaying the dependences of the probe contact electric current on both the probe potential and the probe pressing force. An original method based on the SPM probe controlled electrical current was proposed for the formation of nanosystems with various electrical properties on the surfaces of thin MO films.

The use of polymers as flocculating additives is a common practice in many manufacturing environments. However, exactly how these polymers interact with surfaces is relatively unknown. One specific topic which is thought to be very important to flocculation is an adsorbed polymer's conformation. Substantial amounts of previous work, mainly using simulations, have been performed to elucidate the theory surrounding adsorbed polymer conformations. Yet, there is little experimental work which directly verifies current theory. In order to optimize the use of polymer flocculants in industrial applications, a better understanding of an adsorbed polymer's conformation on a surface beyond theoretical simulations is necessary. This work looks specifically at site blocking, which has a broad impact on flocculation, adsorption, and surface modification, and investigated its effects on the resulting adsorbed polymer conformation. Experimental methods which would allow direct determination of adsorbed polymer conformational details and be comparable with previous experimental results were first determined or developed. Characterization of an adsorbed polymer's conformation was then evaluated using dynamic light scattering, a currently accepted experimental technique to examine this. This commonly used technique was performed to allow the comparison of this works results with past literature. Next, a new technique using atomic force microscopy was developed, building on previous experimental techniques, to allow the direct determination of an adsorbed polymer's loop lengths. This method also was able to quantify changes in the length of adsorbed polymer tails. Finally, mesoscopic simulation was attempted using dissipative particle dynamics. In order to determine more information about an adsorbed polymer's conformation, three different environmental factors were analyzed: an adsorbed polymer on a surface in water, an adsorbed polymer on a surface in aqueous solutions of varying ionic strength, and an adsorbed polymer on a surface functionalized with site blocking additives. This work investigated these scenarios using a low charge density high molecular weight cationic polyacrylamide. Three different substrates, for polymer adsorption were analyzed: mica, anionic latex, and glass. It was determined that, similar to previous studies, the adsorbed polymer layer thickness in water is relatively small even for high molecular weight polymers, on the order of tens of nanometers. The loop length distribution of a single polymer, experimentally verified for the first time, revealed a broad span of loop lengths as high as 1.5 microns. However, the bulk of the distribution was found between 40 and 260 nanometers. For the first time, previous theoretical predictions regarding the salt effect on adsorbed polymer conformation were confirmed experimentally. It was determined that the adsorbed polymer layer thickness expanded with increasing ionic strength of the solvent. Using atomic force microscopy, it was determined that the adsorbed polymer loop lengths and tail lengths increased with increasing ionic strength, supporting the results found using dynamic light scattering. The effect of the addition of site blocking additives on a single polymer's conformation was investigated for the first time. It was determined that the addition of site blocking additives caused strikingly similar results as the addition of salt to the medium. The changes in an adsorbed polymer's loop lengths was found to be inconsistent and minimal. However, the changes in an adsorbed polymer's free tail length was found to increase with increasing site blocking additive levels. These results were obtained using either PDADMAC or cationic nanosilica as site blocking additives.

L'augmentation des performances des circuits intégrés s'est effectué durant les trentes dernières années par la miniaturisation du composant clé à savoir le transistor MOSFET. Cette augmentation de la densité d'intégration se heurte aujourd'hui à plusieurs verrous, notamment celui de la puissance consommée qui devient colossale. Il devient alors nécessaire de travailler sur de nouveaux composants, les transistors à effet tunnel, où les porteurs sont injectés par effet tunnel bande à bande permettant de limiter considérablement la puissance consommée en statique. Les nanofils semiconducteurs sont de bons candidats pour être intégrés comme canaux de ces nouveaux composants de part la possibilité de moduler leur gap et leur conductivité au cours de la croissance. Dans ce contexte, cette thèse traite de la croissance d'hétérostructures axiales Si/Si1-xGex élaborés par croissance VLS par RP-CVD. Tout d'abord, nous identifions les conditions de croissance pour réaliser des interface Si/Si1-xGex et Si1-xGex/Si abruptes. Les deux heterointerfaces sont toujours asymétrique quelle que soit la concentration en Ge ou le diamètre des nanofils ou des conditions de croissance. Deuxièmement, nous étudions les problématiques impliquées par l'ajout d'atomes dopants. Nous discutons de l'influence des paramètres de croissance (le rapport flux de gaz (Si / Ge), et la pression partielle de dopants) sur la morphologie des nanofils et la concentration de porteurs. Grâce à cette étude, nous avons été capable de faire croitre des hétérojonctions P-I-N. Troisièmement, nous présentons une technique basée sur la microscopie à sonde locale pour caractériser les hétérojonctions. / After more than 30 years of successful scaling of MOSFET for increasing the performance and packing density, several limitations to further performance enhancements are now arising, power dissipation is one of the most important one. As scaling continues, there is a need to develop alternative devices with subthreshold slope below 60 mV/decade. In particular, tunnel field effect transistors, where the carriers are injected by quantum band to band tunneling mechanism can be promising candidate for low-power design. But, such devices require the implementation of peculiar architectures like axial heterostructured nanowires with abrupt interface. Using Au catalyzed vapor-liquid-solid synthesis of nanowires, reservoir effect restrains the formation of sharp junctions. In this context, this thesis addresses the growth of axial Si and Si1-xGex heterostructured nanowire with controlled interfacial abruptness and controlled doping using Au catalyzed VLS growth by RP-CVD. Firstly, we identify the growth conditions to realize sharp Si/Si1-xGex and Si1-xGex/Si interfacial abruptness. The two heterointerfaces are always asymmetric irrespective of the Ge concentration or nanowire diameter or growth conditions. Secondly, we study the problematics involved by the addition of dopant atoms and focus on the different approaches to realize taper free NWs. We discuss the influence of growth parameters (gas fluxes (Si or Ge), dopant ratio and pressure) on NW morphology and carrier concentration. With our growth process, we could successfully grow p-I, n-I, p-n, p-i-n type junctions in NWs. Thirdly, we present scanning probe microscopy to be a potential tool to delineate doped and hetero junctions in these as-grown nanowires. Finally, we will integrate the p-i-n junction in the NW in omega gate configuration.

Le composé intermétallique ordonné Ni3Al, de structure L12, présente une augmentation de contrainte d'écoulement avec la température, jusqu'à une température dite de "pic" au-delà de laquelle celle-ci décroit. Ce comportement, usuellement appelé anomalie de contrainte d'écoulement, est mis à profit dans les superalliages base nickel pour les applications hautes températures. Il a été étudiée de façon extensive ces trente dernières années et a donné lieu à de nombreuses modélisations. La plupart des modèles proposés considère qu'un processus thermiquement activé de glissement dévié des dislocations, à partir de leur plan de glissement primaire {111} sur le plan cubique de déviation {010}, joue un rôle clé dans la compréhension de l'anomalie. La distance de glissement dévié peut cependant fortement différer. Les traces de glissement laissées par l'émergence des dislocations mobiles à la surface d'échantillons déformés plastiquement permettent de visualiser les événements de déviations et de caractériser les mécanismes élémentaires de déformation plastique. Nous avons mesuré des paramètres essentiels pour modéliser la plasticité globale de l'intermétallique Ni3Al, comme : le nombre, la hauteur, la longueur des traces de glissement correspondant aux plans {111} et {010}. Ces paramètres qui caractérisent à la fois l'activité des sources et le libre parcours moyen des dislocations, suggèrent que l'anomalie s'accompagne d'un fort taux d'épuisement de la densité de dislocations mobiles. De nombreuses longues déviations dans les plans {010} ainsi que des doubles glissement dévié entre plans {111} adjacents, ont été mis en évidence. Ceci suggère deux processus de glissement dévié. / Ni3Al intermetallic compounds, that correspond to the strengthening phase of nickel-based superalloys, are well known to exhibit within a given range of temperature, an anomalous behaviour of flow strength. This positive temperature dependence of flow strength, called yield stress anomaly (YSA), has been the subject of extensive experimental studies concerning mechanical properties and dislocation microstructures, which have yielded several plausible models. Most of these models considers that a thermally activated cross-slip process, from the primary {111} onto the cube cross-slip {010} planes, plays a key role in the understanding of the YSA. However, the height of the cross-slipped segment in the {010} plane can be drastically different. The slip traces resulting from the emergence of moving dislocations at the surface in plastically deformed samples, allow us to visualize cross-slip events and to characterize the elementary mechanisms controlling plastic deformation. The number, height and length of slip traces corresponding to {111} and {010} planes, that are key parameters for modelling the plastic behaviour of Ni3Al intermetallic, are examined. These parameters reflect both the source activity and dislocation mean free path of dislocations; their values suggest that the YSA takes place with a strong exhaustion of mobile dislocations. Several larger deviations on the {010} planes, as well as double cross-slip between {111} neighbouring planes, are highlighted. These results suggest two different cross-slip process.

Kyoto University (京都大学) / 0048 / 新制・課程博士 / 博士(工学) / 甲第14572号 / 工博第3040号 / 新制||工||1453(附属図書館) / 26924 / UT51-2009-D284 / 京都大学大学院工学研究科材料工学専攻 / (主査)教授 杉村 博之, 教授 酒井 明, 准教授 山田 啓文 / 学位規則第4条第1項該当

The work of this thesis comprises extensive Noncontact Atomic Force Microscopy (NC-AFM) characterization of clean metal-oxide (YSZ(100)/(111) and MgO(100)) and graphitic (HOPG) supports as templates for the novel, photochemically induced nucleation of cobalt oxide nanostructures, particularly Cobalt (III) Oxide. The nanostructure-support surfaces were also studied by X-ray Photoelectron Spectroscopy (XPS) to verify the nature of the supported cobalt oxide and to corroborate the surface topographic and phase NC-AFM data. Heteroepitaxial growth of Co2O3 nanostructures proves to exhibit a variety of different growth modes based on the structure of the support surface. On this basis, single-crystal support surfaces ranging from nonpolar to polar and atomically flat to highly defective and reactive were chosen, again, yielding numerous substrate-nanostructure interactions that could be probed by high-performance surface science techniques.