Hierarchically porous nitrogen-doped graphene frameworks (N-GFs) are fabricated through the ice-templating of GO with polyethylenimine and the thermal treatment of the resultant hybrids. As cathode materials in lithium ion batteries (LIBs), the obtained N-GFs exhibit an outstanding specific capacity of 379 mA h g−1 at 0.5 A g−1 for 2500 cycles. Even at an ultrahigh current density of 5 A g−1, the N-GFs maintain a capacity of 94 mA h g−1, superior to that of most reported LIB cathode materials. The experimental results and quantum mechanics calculations suggest that pyridinic-like N and pyridinic N-oxide in graphene are responsible for the excellent cathodic performance of the bipolar N-GFs by providing fast surface faradaic reactions with both p- and n-doped states.

Hierarchically porous nitrogen-doped graphene frameworks (N-GFs) are fabricated through the ice-templating of GO with polyethylenimine and the thermal treatment of the resultant hybrids. As cathode materials in lithium ion batteries (LIBs), the obtained N-GFs exhibit an outstanding specific capacity of 379 mA h g−1 at 0.5 A g−1 for 2500 cycles. Even at an ultrahigh current density of 5 A g−1, the N-GFs maintain a capacity of 94 mA h g−1, superior to that of most reported LIB cathode materials. The experimental results and quantum mechanics calculations suggest that pyridinic-like N and pyridinic N-oxide in graphene are responsible for the excellent cathodic performance of the bipolar N-GFs by providing fast surface faradaic reactions with both p- and n-doped states.

Two gas-phase ion-molecule reaction systems are presented here based on measurements done in a temperature variable 22-pole trapping machine. In the first case, the proton affinity of methane is determined based on a new technique for measuring the equilibrium constant of the HCO2+ + CH4 <=> CH5+ + CO2 reaction. The second case reports to the (Ar + N2 )+ reaction system, with reaction rate temperature dependencies measurements made both in the forward and reverse direction with different and complementary methods. The temperature variable 22-pole trapping machine allows one to determine equilibrium constants and reaction rate coefficients over a wide range of temperatures. The coupling of an effusive beam to the setup overcomes the problem of neutral gas wall condensation and extends the temperature range measurements beyond condensation point. The introduction (Chapter 1) gives a short overview about the rf technology and parallel experimental techniques developed in order to better characterize and understand the several mechanisms related to ion-molecule reactions. It also focuses some aspects of reaction rate temperature dependencies determination as well as thermodynamical equilibrium in laboratory environment. A short description of the setup and experimental methods are presented in Chapter 2. Based on equilibrium constant measurements, Chapter 3 is dedicated to the proton affinity of methane. This concept has applications on several fields such as atmospheric and combustion modelling, or testing empirical and ab initio theories for electronic structures. The (Ar − N2 )+ system presented in Chapter 4, is known for being a good case study for inferring the role of vibrational excitation in reaction dynamics and to the existence of non-adiabatic coupling. The experimental results here presented for the N2+ + Ar reaction demonstrate that it is possible to avoid parallel reactions with first vibrational excited state of nitrogen (N2 (ν = 1)). On the other hand, the reverse reaction experiments confirm the existence of a minimum of the reaction rate in the 30 to 300 K range, due to the existence of two reaction channels. The question of the high rate coefficient towards lower temperatures being related to the N2 rotational ground state population is raised. A summary and outlook are presented in Chapter 5, where some new possible paths of investigation are pointed out.

Eine der drei Säulen der Krebsbehandlung ist die Strahlentherapie. Einer der neuesten Ansätze hierbei ist die Bestrahlung mit Ionen, zurzeit insbesondere Protonen und Kohlenstoffionen. Diese Hochpräzisionstherapie erfordert ein hohes Maß an Kontrolle, da die applizierte Dosisverteilung sehr empfindlich von Dichteveränderungen im durchstrahlten Gewebe abhängt. Das bisher einzige klinisch eingesetzte Verfahren zur in vivo Überwachung der Dosisapplikation bei Ionenbestrahlungen ist die Positronen-Emissions-Tomographie (PET). Sie ermöglicht eine Verifikation der Teilchenreichweite sowie der Lage des Bestrahlungsfeldes. Die mit der PET-Methode gemessene Aktivitätsverteilung lässt sich jedoch nicht direkt mit der geplanten Dosisverteilung vergleichen. Daher ist eine Vorherberechnung der erwarteten Aktivitätsverteilung auf der Grundlage des Bestrahlungsplanes notwendig, welche dann mit der Messung verglichen wird und eine qualitative Beurteilung der Bestrahlung ermöglicht. Die Vorherberechnung der erwarteten Aktivitätsverteilung erfordert bislang die Kenntnis einer Vielzahl von Wirkungsquerschnitten. Nur für wenige dieser Wirkungsquerschnitte liegen jedoch Messdaten im benötigten Energiebereich und mit ausreichender Genauigkeit vor. Daher verwenden viele Monte-Carlo-Simulationen intrinsische Kernmodelle oder semi-empirische Modellierungen, die häufig eine unzureichende Genauigkeit aufweisen. In Fachkreisen ist bisher noch nicht geklärt, welches die optimale Ionensorte für die Tumortherapie ist. Insbesondere Lithiumionen weisen aufgrund ihrer physikalischen und radiobiologischen Eigenschaften ein großes Potenzial auf. Auch für Bestrahlungen mit diesen Ionen ist ein PET-Monitoring der Therapie erstrebenswert. In der vorliegenden Arbeit wird zunächst die Anwendbarkeit der Reichweite-Verifikation mittels PET bei Bestrahlung mit Lithiumionen gezeigt. Des Weiteren wird ein Konzept zur Modellierung der Positronenemitter-Verteilung ohne Kenntnis der Wirkungsquerschnitte entwickelt. Diese Vorhersage beruht auf in Referenzmaterialien (Wasser, Graphit und Polyethylen) gemessenen tiefenabhängigen Positronenemitter-Yields, mit welchen durch geeignete Linearkombination die Verteilung der Positronenemitter in beliebigen Materialien bekannter Stöchiometrie vorausberechnet werden kann. Die Anwendbarkeit des Yield-Konzeptes wird gezeigt für Lithium- und Kohlenstoffbestrahlungen homogener Polymethylmethacrylat (PMMA) Targets sowie verschiedener inhomogener Targets. / One of the three main tumour treatment forms is radiation therapy. Here, the application of ion beams, in particular protons and carbon ions, is of growing importance. This high precision therapy requires a consequent monitoring of the dose delivery since the induced dose deposition is very sensitive to density changes in the irradiated tissue. Up to now, positron emission tomography (PET) is the only in vivo method in clinical use for monitoring the dose deposition in ion beam therapy. It allows for the verification of the particle range as well as the position of the irradiation field. The distribution of activity measured by means of PET cannot be compared directly to the planned dose distribution. Thus, a calculation of the expected activity distribution is required which then can be compared to the measurement. Simulation of the expected activity distribution requires the exact knowledge of various cross sections. Only a few of them have been measured in the required energy range so far. Therefore, in Monte Carlo simulations often intrinsic nuclear models or semi-empirical parametrization are used which often exhibit insufficient accuray. Among experts the question on the optimum ion species for tumour therapy is still open. Especially lithium ions exhibit a great potential due to their favourable physical and radiobiological properties. Also for these ions a PET monitoring is highly desirable. The presented work shows the feasibility of range verification by means of PET for lithium irradiation. Furthermore, a concept for modeling positron emitter distributions without the knowledge of cross sections is developed. This prediction is based on depth-dependent positron emitter yields measured in reference materials (water, graphite and polyethylene). With these data the positron emitter distribution in any material of known stoichiometry can be calculated by means of an appropriate linear combination. The feasibility of the yield concept is shown for lithium and carbon irradiation, respectively, of homogeneous polymethyl methacrylate (PMMA) as well as various inhomogeneous targets.

In this work, atomic scale investigation of pressure-induced transformations in the solid state have been carried out. A series of compounds including GaN, ZnO, CaF2, and AgI, in addition to elemental phosphorus have been studied. The corresponding transition mechanisms have been elucidated with a clear description of atomic displacements and intermediate structures involved therein. In the first group of compounds, the long standing debate on the transition path of the wurtzite(WZ)-to-rocksalt(RS) transition in semiconductors, GaN and ZnO was resolved using geometrical modeling combined with molecular dynamics (MD) simulations conducted in the frame of transition path sampling (TPS) method. In GaN, a two-step mechanism through a metastable intermediate phase with a tetragonal structure iT has been revealed from simulations. In ZnO, the tetragonal intermediate structure was kinetically less stable, although still part of the real transition mechanism. It appeared at the interface between WZ and RS as consequence of a layers shearing. The transition regime in ZnO was characterized by a competition between iT structure and another hexagonal intermediate with hexagonal symmetry iH. Although possible, the latter is not functional for the transition. In both cases, GaN and ZnO, two points of agreement with experiments have been revealed. The tilting of structures after transition, and the phonon mode softening associated with atomic displacements leading to the tetragonal structure iT In the second group of compounds, the investigation of transitions in superionic conductors, CaF2 and AgI, demonstrated a different and particular behavior of atomic motion under pressure. The solid-solid reconstruction of CaF2 structure was shown to be initiated and precedented by high disorder of the anionic sublattice. The percolation of fluoride ions through voids in the fluorite structure created a thin interface of liquid like state. The sparce regions caused by the departure of anions facilitates the cation sublattice reconstruction. In AgI, ion diffusion during the wurtzite/zincnlende(ZB)$rocksalt transition was more pronounced due to the extended stacking disorder WZ/ZB. The Ag+ ions profited not only from the structure of the interface but used the combination of interstitial voids offered by both phases, WZ and ZB, to achieve long diffusion paths and cause the cation sublattice to melt. Clearly, a proper account for such phenomena cannot be provided by geometry-designed mechanisms based on symmetry arguments. In phosphorus, the question of how the stereochemically active lone pairs are reorganized during the orthorhombic (PI) to trigonal (PV) structural transition was answered by means of simulations. Computation was performed at different levels theory. First, the mechanism of the transition was obtained from TPS MD simulations. MD runs were performed within density functional tight binding method (DFTB). The analysis of atomic displacements along the real transformation path indicated a fast bond switching mechanism. In a second step, the nature of the interplay between orbitals of phosphorus during the bond switching was investigated. A simultaneous deformation of lone pair and P−P bond showed a mutual switching of roles during the transformation. This interplay caused a low dimensional polymerization of phosphorus under pressure. The corresponding structure formed as zigzag linear chain of fourfold coordinated phosphorus atoms (· · ·(P(P2))n · · ·) at the interface between PI and PV phases. A further result of this work was the development of a simulation strategy to incorporate defects and chemical doping to structural transformations. On top of the transition path sampling iterations, a Monte Carlo like procedure is added to stepwise substitute atoms in the transforming system. Introducing a chemically different dopant to a pure system represents a perturbation to the energy landscape where the walk between different phases is performed. Therefore, any change in the transition regime reflects the kinetic preference of a given structural motif at times of phase formation. This method was applied to the elucidation of WZ-RS transition mechanism in the series of semiconducting compounds AlN, GaN, and InN. Simulations showed that In atoms adopt the same transformation mechanism as in GaN and favor it, while Al atoms demonstrated a significant reluctance to the path going through tetragonal intermediate iT. The difference between transition regime in mixed systems InxGa1−xN and AlxGa1−xN is in agreement with experiments on high pressure behavior of AlN, GaN, and InN. While transitions in GaN and InN are reversible down to ambient conditions, AlN is stable. The work presented in this thesis constitutes the seed of new perspectives in the understanding of pressure-induced phase transformations in the solid state, where the physics and the chemistry are brought together by means of computer simulations.

Lithium ion batteries (LIBs) have attracted considerable interest due to their wide range of applications, such as portable electronics, electric vehicles (EVs) and aerospace applications. Particularly, the emergence of a variety of nanostructured materials has driven the development of LIBs towards the next generation, which is featured with high specific energy and large power density. Herein, rolled-up nanotechnology is introduced for the design of strain-released materials as anodes of LIBs. Upon this approach, self-rolled nanostructures can be elegantly combined with different functional materials and form a tubular shape by relaxing the intrinsic strain, thus allowing for enhanced tolerance towards stress cracking. In addition, the hollow tube center efficiently facilitates electrolyte mass flow and accommodates volume variation during cycling. In this context, such structures are promising candidates for electrode materials of LIBs to potentially address their intrinsic issues. This work focuses on the development of superior structures of Si and SnO2 for LIBs based on the rolled-up nanotech. Specifically, Si is the most promising substitute for graphite anodes due to its abundance and high theoretical gravimetric capacity. Combined with the C material, a Si/C self-wound nanomembrane structure is firstly realized. Benefiting from a strain-released tubular shape, the bilayer self-rolled structures exhibit an enhanced electrochemical behavior over commercial Si microparticles. Remarkably, this behavior is further improved by introducing a double-sided carbon coating to form a C/Si/C self-rolled structure. With SnO2 as active material, an intriguing sandwich-stacked structure is studied. Furthermore, this novel structure, with a minimized strain energy due to strain release, exposes more active sites for the electrochemical reactions, and also provides additional channels for fast ion diffusion and electron transport. The electrochemical characterization and morphology evolution reveal the excellent cycling performance and stability of such structures.

Die Menschheit steht vor der großen Herausforderung der Energieversorgung des 21. Jahrhundert. Nirgendwo ist diese noch dringlicher geworden als im Bereich der Energiespeicherung und Umwandlung. Konventionelle Energie kommt hauptsächlich aus fossilen Brennstoffen, die auf der Erde nur begrenzt vorhanden sind, und hat zu einer starken Belastung der Umwelt geführt. Zusätzlich nimmt der Energieverbrauch weiter zu, insbesondere durch die rasante Verbreitung von Fahrzeugen und verschiedener Kundenelektronik wie PCs und Mobiltelefone. Alternative Energiequellen sollten vor einer Energiekrise entwickelt werden. Die Gewinnung erneuerbarer Energie aus Sonne und Wind sind auf jeden Fall sehr wichtig, aber diese Energien sind oft nicht gleichmäßig und andauernd vorhanden. Energiespeichervorrichtungen sind daher von großer Bedeutung, weil sie für eine Stabilisierung der umgewandelten Energie sorgen. Darüber hinaus ist es eine enttäuschende Tatsache, dass der Akku eines Smartphones jeglichen Herstellers heute gerade einen Tag lang ausreicht, und die Nutzer einen zusätzlichen Akku zur Hand haben müssen. Die tragbare Elektronik benötigt dringend Hochleistungsenergiespeicher mit höherer Energiedichte. Der erste Teil der vorliegenden Arbeit beinhaltet Lithium-Ionen-Batterien unter Verwendung von einzelnen aufgerollten Siliziumstrukturen als Anoden, die durch nanotechnologische Methoden hergestellt werden. Eine Lab-on-Chip-Plattform wird für die Untersuchung der elektrochemischen Kinetik, der elektrischen Eigenschaften und die von dem Lithium verursachten strukturellen Veränderungen von einzelnen Siliziumrohrchen als Anoden in einer Lithium-Ionen-Batterie vorgestellt. In dem zweiten Teil wird ein neues Design und die Herstellung von flexiblen on-Chip, Festkörper Mikrosuperkondensatoren auf Basis von MnOx/Au-Multischichten vorgestellt, die mit aktueller Mikroelektronik kompatibel sind. Der Mikrosuperkondensator erzielt eine maximale Energiedichte von 1,75 mW h cm-3 und eine maximale Leistungsdichte von 3,44 W cm-3. Weiterhin wird ein flexibler und faserartig verwebter Superkondensator mit einem Cu-Draht als Substrat vorgestellt. Diese Dissertation wurde im Rahmen des Forschungsprojekts GRK 1215 "Rolled-up Nanotechnologie für on-Chip Energiespeicherung" 2010-2013, finanziell unterstützt von der International Research Training Group (IRTG), und dem PAKT Projekt "Elektrochemische Energiespeicherung in autonomen Systemen, no. 49004401" 2013-2014, angefertigt. Das Ziel der Projekte war die Entwicklung von fortschrittlichen Energiespeichermaterialien für die nächste Generation von Akkus und von flexiblen Superkondensatoren, um das Problem der Energiespeicherung zu addressieren. Hier bedanke ich mich sehr, dass IRTG mir die Möglichkeit angebotet hat, die Forschung in Deutschland stattzufinden. / Human beings are facing the grand energy challenge in the 21st century. Nowhere has this become more urgent than in the area of energy storage and conversion. Conventional energy is based on fossil fuels which are limited on the earth, and has caused extensive environmental pollutions. Additionally, the consumptions of energy are still increasing, especially with the rapid proliferation of vehicles and various consumer electronics like PCs and cell phones. We cannot rely on the earth’s limited legacy forever. Alternative energy resources should be developed before an energy crisis. The developments of renewable conversion energy from solar and wind are very important but these energies are often not even and continuous. Therefore, energy storage devices are of significant importance since they are the one stabilizing the converted energy. In addition, it is a disappointing fact that nowadays a smart phone, no matter of which brand, runs out of power in one day, and users have to carry an extra mobile power pack. Portable electronics demands urgently high-performance energy storage devices with higher energy density. The first part of this work involves lithium-ion micro-batteries utilizing single silicon rolled-up tubes as anodes, which are fabricated by the rolled-up nanotechnology approach. A lab-on-chip electrochemical device platform is presented for probing the electrochemical kinetics, electrical properties and lithium-driven structural changes of a single silicon rolled-up tube as an anode in lithium ion batteries. The second part introduces the new design and fabrication of on chip, all solid-state and flexible micro-supercapacitors based on MnOx/Au multilayers, which are compatible with current microelectronics. The micro-supercapacitor exhibits a maximum energy density of 1.75 mW h cm-3 and a maximum power density of 3.44 W cm-3. Furthermore, a flexible and weavable fiber-like supercapacitor is also demonstrated using Cu wire as substrate. This dissertation was written based on the research project supported by the International Research Training Group (IRTG) GRK 1215 "Rolled-up nanotech for on-chip energy storage" from the year 2010 to 2013 and PAKT project "Electrochemical energy storage in autonomous systems, no. 49004401" from 2013 to 2014. The aim of the projects was to design advanced energy storage materials for next-generation rechargeable batteries and flexible supercapacitors in order to address the energy issue. Here, I am deeply indebted to IRTG for giving me an opportunity to carry out the research project in Germany. September 2014, IFW Dresden, Germany Wenping Si

Die vorliegende Arbeit liefert einen Beitrag zum Verständnis der elektrochemischen Prozesse an der Elektrodengrenzfläche und im Festkörper graphitischer Anoden für Lithium-Ionen-Batterien. Der Zusammenhang zwischen den intrinsischen Eigenschaften des Aktivmaterials und den resultierenden Eigenschaften von Kompositelektroden stand dabei im Fokus der Untersuchungen. Die Temperaturabhängigkeit von Materialeigenschaften (Diffusionskoeffizient, Austauschstromdichte) und Elektrodeneigenschaften (Verhalten unter Strombelastung) wurde in einem Bereich von 40 °C bis -10 °C erfasst. Dazu werden elektrochemische Charakterisierungsmethoden aus der Literatur vorgestellt und hinsichtlich ihrer Gültigkeit für die Anwendung an realen Elektroden evaluiert. Die elektrochemisch aktive Oberfläche wurde bestimmt und stellte sich als ausschlaggebender Parameter für die Bewertung der Elektrodenprozesse heraus. Auf Basis korrigierter Elektrodenoberflächen konnten Austauschstromdichten für die konkurrierenden Prozesse Lithium-Interkalation und -Abscheidung ermittelt werden. Zusammen mit Kennwerten zur Keimbildungsüberspannung für Lithium-Abscheidung flossen die ermittelten Kennwerte in eine theoretische Berechnung des Zellstroms ein. Es konnte gezeigt werden, dass die Lithium-Abscheidung kinetisch deutlich gegenüber der Lithium-Interkalation bevorzugt ist, nicht nur bei niedriger Temperatur. Die Übertragbarkeit wissenschaftlicher Grundlagenexperimente auf kommerzielle Systeme war bei allen Versuchen Gegenstand der Untersuchungen. In einem separaten Beispiel einer Oberflächenmodifikation mit Zinn wurde diese Problematik besonders verdeutlicht. Zusätzlich wurde die parasitäre Abscheidung von Lithium auf graphitischen Anoden hinsichtlich der Nachweisbarkeit und Quantifizierung evaluiert. Hierfür wurde eine neue Untersuchungsmethode im Bereich der Lithium-Ionen-Batterie zur besseren Detektion von Lithium-Abscheidung und Grenzflächen-Morphologie mittels Elektronenmikroskopie entwickelt. Die Osmiumtetroxid (OsO4) Färbung ermöglichte eine deutliche Verbesserung des Materialkontrasts und erlaubte somit eine gezielte Untersuchung von graphitischen Anoden nach erfolgter Lithium-Abscheidung. Darüber hinaus konnte die selektive Reaktion des OsO4 für eine genauere Betrachtung der Solid Electrolyte Interphase genutzt werden. Eine Stabilisierung der Proben an Luft und im Elektronenstrahl konnte erreicht werden. / This work sheds light on the electrochemical processes occurring at commercially processed graphitic anodes. It raises the question whether values published in literature for mostly ideal electrode systems can be readily taken for simulation and design of real electrodes in high-energy cells. A multiple step approach is given, evaluating different methods to determine electrode and material properties independently. The electrochemically active surface area was shown to be a crucial parameter for the calculation of electrode kinetics. Using exchange current densities corrected for the electrode surface area, the overall charging current in a cell could be calculated. The resulting part of lithium deposition in the charging process is strikingly high, not only at low temperatures. To further investigate lithium deposition in terms of morphology and quantity, a method was developed for graphitic anodes. Osmium tetroxide (OsO4) staining serves well as a tool to strongly increase material contrast in electron microscopy. Thus lithium dendrites could be made visible in an unprecedented manner. Furthermore, the selective chemical reaction of osmium tetroxide allows for a better investigation of the multi-layer solid electrolyte interphase as was shown in transmission electron microscopy. Using the staining method, a stabilization of the sample under air and in the electron beam could be achieved.

As an efficient energy storage technology, lithium-ion batteries play a key role in the ongoing electrification of the mobility sector. However, the required modelbased design process, including hardware in the loop solutions, demands precise battery models. In this work, an encoder-decoder model framework based on recurrent neural networks is developed and trained directly on unstructured battery data to replace time consuming characterisation tests and thus simplify the modelling process. A manifold pseudo-random bit stream dataset is used for model training and validation. A mean percentage error (MAPE) of 0.30% for the test dataset attests the proposed encoder-decoder model excellent generalisation capabilities. Instead of the recursive one-step prediction prevalent in the literature, the stage-wise trained encoder-decoder framework can instantaneously predict the battery voltage response for 2000 time steps and proves to be 120 times more time-efficient on the test dataset. Accuracy, generalisation capability and time efficiency of the developed battery model enable a potential online anomaly detection, power or range prediction. The fact that, apart from the initial voltage level, the battery model only relies on the current load as input and thus requires no estimated variables such as the state-of-charge (SOC) to predict the voltage response holds the potential of a battery ageing independent LIB modelling based on raw BMS signals. The intrinsically ageingindependent battery model is thus suitable to be used as a digital battery twin in virtual experiments to estimate the unknown battery SOH on purely BMS data basis.

Die vorliegende Arbeit entstand im Rahmen einer Kooperation des Forschungszentrums Dresden-Rossendorf mit Qimonda Dresden GmbH & Co. OHG. Mithilfe der hochauflösenden Rutherford-Streuspektrometrie (HR-RBS) wurden das Diffusionsverhalten und Schichtwachstum von ZrO2 auf SiO2 und TiN im Anfangsstadium untersucht. Auf Grund der exzellenten Tiefenauflösung von 0,3 nm an der Oberfläche stand die Analyse von Konzentrationsprofilen in ultradünnen Schichten, respektive an deren Grenzflächen im Vordergrund. Zur qualitativen Verbesserung der Messergebnisse wurde erstmals ein zweidimensionaler positionsempfindlicher Halbleiterdetektor in den Aufbau der HR-RBS implementiert und charakterisiert. Außerdem wurde ein Messverfahren in Betrieb genommen, das mögliche Schädigungen durch den Ioneneintrag in die Messprobe minimiert. Durch die Optimierung der experimentellen Bedingungen und die Entwicklung eines Programmpaketes zur Unterstützung des Analysten konnte ein effizienter Routine-Messablauf erstellt werden. Im Moment einer binären Kollision zwischen einfallendem Ion und Targetelement kommt es bei kleinem Stoßparameter zu Veränderungen des Ladungszustands der gestreuten Ionen, insbesondere durch die abrupte Geschwindigkeitsänderung des Projektils und der Überlappung der Elektronenwolken. Bei der HR-RBS mit Energie separierendem Dipolmagneten muss zur Interpretation von Streuspektren die Ladungszustandsverteilung der gestreuten Projektile bekannt sein. Erstmalig konnte eine signifikante Abhängigkeit der Ladungszustandsverteilung gestreuter C-Ionen sowohl von der Schichtdicke als auch der Ordnungszahl des detektierten Targetelements, hier der vierten Nebengruppe, nachgewiesen werden. Diese gewonnen Erkenntnisse ermöglichten systematische Untersuchungen zum ZrO2-Schichtwachstum im Anfangsstadium. Zur Herstellung der ZrO2-Schichten wurde die Atomlagenabscheidung (ALD) verwendet. Anhand der nachgewiesenen Agglomeration von ZrO2 auf nativen SiO2 wurde mithilfe der Rasterkraftmikroskopie (AFM) zur Bestimmung von Oberflächenrauigkeiten eine Methode konzipiert, welche die Auswirkung lokaler Schichtdickeninhomogenitäten auf die niederenergetische Flanke eines Streuspektrums berücksichtigt. Auf dieser Grundlage durchgeführte Simulationsrechnungen ergeben, dass keine Diffusion von Zr in die darunter liegende Schicht stattfand, jedoch eine ZrSiO4-Grenzflächenschicht existiert. Für das Wachstum von ZrO2 auf TiN wird aus den hoch aufgelösten Streuspektren ein völlig anderes Verhalten abgeleitet. Messungen zu Oberflächentopografien der TiN-Schicht liefern nicht zu vernachlässigende Werte für die Rauigkeit. Um den Einfluss der Oberflächenrauigkeit auf die Form des hoch aufgelösten Spektrums erfassen zu können, wurde eine Software entwickelt. Auf Basis von AFM-Messungen ermöglicht dieses Programm das Extrahieren einer Energieverteilung aus den Weglängen von ausschließlich an der Oberfläche gestreuten Ionen. Unter Berücksichtigung des Effekts der Oberflächenrauigkeit auf die HR-RBS Spektrenform konnte die Diffusion von Zr in das polykristalline TiN erstmals verifiziert werden. Die Beobachtungen weisen daraufhin, dass bereits nach dem ersten ALD-Zyklus ein geringer Anteil der deponierten Zr-Atome bis in eine Tiefe von etwa 3 nm in das TiN diffundiert. Die vorläufigen Ergebnisse legen Korngrenzendiffusion nahe. / This thesis originated from a cooperation between Research Center Dresden-Rossendorf and Qimonda Dresden GmbH & Co. OHG. By means of High Resolution Rutherford Backscattering Spectrometry (HR-RBS) the diffusion behaviour and layer growth of ZrO2 on SiO2 and TiN in the initial regime were investigated. The analysis of concentration profiles in ultrathin layers and interfaces was the focus of this work, made possible by the excellent depth resolution of less than 0.3 nm near the surface. For the first time a two-dimensional position sensitive semiconductor detector was implemented and characterized in the setup of the HR-RBS for the improvement of the quality of the measurement results. Furthermore, a measurement procedure was put into operation that allowed the reduction of ion induced damage. Through the optimization of the experimental conditions and the development of a program package for the support of the analyst, an efficient measurement procedure could be routinely ensured. At the time of a binary collision between the incident ion and the target element with a small impact factor, the charge state changes frequently, especially due to the abruptly decreasing ion velocity of the projectile and the overlapping of the electron clouds. For HR-RBS with an energy-separating dipole magnet, the charge state distribution of the scattered ions must be known for the interpretation of the measured spectra. For the first time a significant dependence of the charge state distribution of the scattered C ions on the layer thickness as well as atomic number of the detected target elements, here from the fourth subgroup, was emonstrated. This new knowledge allowed systematic investigations of the ZrO2 layer growth in the initial regime. The ZrO2 layers were produced by means of the atomic layer deposition (ALD). Based on the evidence for agglomeration of ZrO2 on SiO2 a method was introduced, which takes local thickness variations into account during the simulation of the HR-RBS spectra. An accurate statement about the ZrO2/SiO2 interface was possible due to the extraction of the thickness variation by the atomic force microscopy (AFM). The boundary surface is sharp except for a small intermediate ZrSiO4 layer and no diffusion of Zr atoms in SiO2 could be detected. A quite different behaviour could be derived from high resolution spectra for the growth of ZrO2 on TiN. Measurements of the surface topography of the TiN layer revealed non negligible values for the surface roughness. A program was developed to capture the influence of the surface roughness on the shape of the high resolution spectrum. This software uses AFM measurements to extract an energy distribution from calculated path length differences for ions scattered at the sample surface. Diffusion of Zr into polycrystalline TiN was demonstrated for the first time taking into account the effect of the surface roughness on the shape of the spectra. This observation indicates that already after the first ALD reaction cycle a small part of the deposited Zr atoms diffuses into the TiN layer up to a depth of 3 nm. Such preliminary results suggest grain boundary diffusion.