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In this thesis wave propagation in the whistler wave frequency range ωci≤ω≤ωce in the linear magnetized plasma experiment VINETA is investigated. The plasma is generated by a helicon antenna and has a diameter of about 10 cm. Whistler waves are launched by a loop antenna with a diameter of 4.5 cm and the fluctuating magnetic field is mapped by Ḃ-probes. Experiments are carried out for plasma parameters γ≤1/ √ 2 under which the only transversal polarized wave according to plane wave dispersion theory is the whistler wave. Due to the small collision frequencies ν≪1 cyclotron damping of whistler waves in this parameter regime is dominant and depends only on the electron plasma-β. The influence of the inhomogeneous plasma profile and excitation by a loop antenna is investigated by measurements of the fluctuating magnetic field perpendicular to the ambient magnetic field in azimuthal and radial axial planes. A mode characterized by the number of wave lengths m in the azimuthal direction is found. The mode structure is modified by the specific shape of the plasma density profile. Profiles with a homogeneous density inside the plasma radius are found to posses a comparably simple mode structure. An agreement in the mode structure of full-wave simulations in three dimensions, including a Gaussian density profile and excitation of the wave by a loop antenna, with the experimental results is found. Conclusions on the spatial structure of the excited mode are drawn using the simulations which predict excitation of an m=2 mode. The wave is found to be ducted within the plasma radius over a wide parameter range. A Helmholtz decomposition of the simulations electric field exhibits the fluctuating space charge as the dominant source for the electric field, while the contribution due to induction is negligible. The magnetic field is given partially by the electron and displacement current. Both contributions to the magnetic field are of the same order of magnitude. The frequency dependency of the excited modes spatial damping increment is investigated using measurements of the magnetic fluctuations along the symmetry axis of the plasma. In order to illustrate the parameter dependency, the electron plasma-β is varied over two orders in magnitude in the range β = 4·10-4 - 2.4·10-2. The experimental result for the spatial damping increment of the mode yields a strong damping for wave frequencies ω/ωce > 0.5 at maximum plasma-β, which shifts to higher frequencies with decreasing β. The parameter dependency of the damping for a fixed frequency is studied in an axial ambient magnetic field gradient. In both cases an excellent agreement between the experimental result and predictions for cyclotron damping from plane wave dispersion theory is found.
The layer-by-layer method is a robust way of surface functionalization using a wide range of materials, e.g. synthetic and natural polyelectrolytes (PEs), proteins and nanoparticles. Thus, this method yields films with applications in diverse areas including biology and medicine. Sequential adsorption of different oppositely charged macromolecules can be used to prepare tailored films with controlled molecular organization. In biomedical research, electrically conductive coatings are of interest. In manuscript 1, we investigated films sequentially assembled from the polycation poly (diallyldimethyl-ammonium) (PDADMA) and modified carbon nanotubes (CNTs), with CNTs serving as the electrically conductive material. We assume that charge transport occurs through CNT contacts. We showed that with more than four CNT/PDADMA bilayers, the electrical conductivity is constant and independent of the number of CNT/PDADMA bilayers. A conductivity up to 4∙10^3 S/m was found. It is possible to control the conductivity with the CNT concentration of the CNT deposition suspension. A higher CNT concentration resulted in thicker CNT/PDADMA bilayers, but in a lower conductivity per bilayer. We suspect that an increased CNT concentration leads to a rapid CNT adsorption without the possibility to rearrange themselves. If PDADMA then adsorbs on the disordered CNTs in the next deposition step, the average thickness of the polymer layer is thicker than on the more ordered CNT layer from the dilute solution. This leads to an increased PE monomer/CNT ratio and lower conductivity. More polycations between the CNT layers leads to less CNT contacts. Thus, the controlled composition of films can be used to fulfill specific requirements.
For many applications of polyelectrolyte multilayers (PEMs), cheap PEs with a broad distribution of molecular weights are used. It was unknown whether the distribution of molecular weights of the PE in the adsorption solution is maintained during the adsorption process and hence in the film. To investigate this, the PSS adsorption solution in article 2 consisted of a binary mixture of short and long poly (styrene sulfonate) (PSS). A good model system to study layered films in terms of composition are PDADMA/PSS multilayers. Neutron reflectivity and in-situ ellipsometry measurements were carried out to determine the PSS composition in the film and the growth regimes. At a mole fraction of long PSS of 5 % or more in solution, the exponential growth (which is characteristic of short PSS) is totally suppressed, and only long PSS is deposited in the resulting multilayer. Variation of adsorption time of PSS showed that short PSS first adsorbs to the surface but is displaced by long PSS. Between 0 and 5 % of long PSS in the adsorption solution exponential growth occurs. The fraction of short PSS in the film continuously decreases with the increase of long PSS in the adsorption solution. In the assembly of films prepared from binary PSS mixtures, the short PSS leaves the film through adsorption/desorption steps both during PSS adsorption and during PDADMA adsorption (as PDADMA/PSS complexes). Both techniques show that the composition of the film does not correspond to that of the deposition solution. The composition and thus the properties of the resulting multilayer are influenced by the choice of adsorption time. Moreover, we conclude that a multilayer grown from a polydisperse polyelectrolyte contains fewer mobile low molecular weight polymers than the deposition solution.
In manuscript 1 and article 2, the composition of multilayers was studied. In manuscript 1 adsorption kinetics were important for the arrangement of CNTs on the surface. In article 2, the adsorption kinetics, i.e. the diffusion of the polyelectrolytes to the surface, was also investigated. In article 3, we investigated the influence of the composition of the film as well as the preparation condition on the mobility of PEs in the film. The molecular weight of the polycation PDADMA and the NaCl concentration of the deposition solution were varied. The vertical PSS diffusion constant D_PSS within the PDADMA/PSS multilayers was measured using neutron reflectivity. The salt concentration of the preparation solution defines the polymer conformation during deposition. The molecular weight of the polycation determines the degree of intertwining. Together, both parameters determine the polyanion-polycation coupling and thus the PSS mobility within the network. Log−log display of D_PSS vs the molecular weight of PDADMA and fits to two power laws (D_PSS ∝ X_n(PDADMA)^(-m) ∝ M_w(PDADMA)^(-m)) reveals for films built from 10 or 200 mM NaCl a kink. Below and above the kink, the dependence of D_PSS on M_w(PDADMA) can be described by different power laws. For Χ_n(PDADMA) < X_n,kink(PDADMA) ≈ 288, the exponents are consistent with the predictions of the sticky reptation model. X_n(PDADMA) ≈ 288 is the entanglement limit. For Χ_n(PDADMA) > X_n,kink(PDADMA) ≈ 288, the decrease of D_PSS with M_w(PDADMA) is larger than below the entanglement limit, which is indicative of sticky reptation and entanglement. The PSS diffusion constant of films built from 100 mM NaCl drops three orders of magnitude when increasing the molecular weight of PDADMA from 45 kDa to 72 kDa. To figure out if an immobile PSS fraction exists in the film built from 72 kDa PDADMA (beyond the entanglement limit), the film was annealed at different conditions in article 4: both temperature and salt concentration were varied. For data analysis, the simplest model with two PSS fractions with different diffusion constants was used. These diffusion constants increase as the temperature of the surrounding solution is increased. As assumed in article 3, an immobile PSS fraction exists when annealing at room temperature. At higher annealing temperatures, at least two diffusion processes must be distinguished: the diffusion of the highly mobile PSS fraction through the entire film and a slow PSS fraction, mowing in a limited way. The choice of preparation conditions determines whether a polyelectrolyte multilayer can intermix completely. It is not clear if complete intermixing will ever occur for films built with PDADMA beyond the entanglement limit. It is possible that the diffusion is more complex. Long-term measurements will clarify this question. Calculating scattering length density profiles with subdiffusive behavior would be interesting and is a challenge for the future. Furthermore, immobile fractions are only visible with long annealing times. We hypothesize that an immobile or nearly immobile fraction is present whenever the dependence of D_PSS on the molecular weight of PDADMA cannot be described by the sticky reptation. To verify this hypothesis, further studies are necessary.
All results presented and discussed in the manuscript and articles show that by varying the preparation conditions, tailored films can be built. The composition of the film is also determined by the adsorption kinetics. In addition, the mobility of the PEs within the multilayers can be controlled by varying the conformation, mingling and entanglement of the chains within the film. The influence of the salt concentration in the preparation solution on the growth regimes during film formation is part of our future research. It is planned to investigate films built of different PDADMA molecular weights under varied annealing conditions to better understand the mobile and immobile fractions.
In this work, the investigation of dusty plasma by means of tunable diode laser spectroscopy was carried out. Special interest was focused on the interactions of dust particles and metastable atoms. At first, Al density and temperature in dc and pulsed magnetron discharges were measured. Measurements with argon as working gas show an expected behavior of the measured atom density and temperature. Decrease of absorption signal was observed in argon/oxygen and argon/methane mixtures. A small admixture of oxygen leads to a complete disappearance of the absorption signal indicating vanishing Al atom density. The effect is believed to be caused by the oxidation of the magnetron target. This decrease reveals typical hysteresis behavior caused by poisoning of the target. Significant difference between critical oxygen flow value in dc and pulsed modes was registered. Then dust formation and plasma behaviors in hydrocarbon containing plasmas were analysed. The dust growing plasmas (Ar/C2H2, Ar/CH4 and Ar/C3H6 rf plasmas) were characterized by laser transmission and scattering methods, ion energy distribution function and mass spectrum evolution by plasma processing monitor, and the spatial distribution in pristine plasma and the temporal behavior of the metastable atom density in processing plasma using TDLAS. Pristine plasma were then characterized in term of metastable density and temperature. The radial distribution of neon metastable atom density in capacitive coupled rf discharge can be approximated to a Gaussian profile with the width smaller than plasma chamber radius. The diffusion flow of metastable atoms deduced from their spatial density distribution gives the loss of metastable atom in the plasma sheath. Argon metastable density was measured in rf plasma and compared with a simple model for metastable density. The model explains well the trend of metastable density with respect to the change of plasma input power. Metastable density of dusty plasma with injected dust particles was measured and compared to that of pristine plasma. The particle heating by metastable atoms was strongly evidenced. The power absorbed by dust particles due to bombardment of metastable atoms onto a dust particle surface in our experiments is about 0.04 Wm-2 for the low dust density case and lower for higher dust density which is in the same order as the contributions of kinetic energy of ions and electrons and the energy released by their recombination on the grain surface. The influence of dust particle density and size on metastable density was studied. Through measuring metastable density, TDLAS can be used as a tool to study the dust growth process in processing plasma.
The confinement of energy has always been a challenge in magnetic confinement fusion devices. Due to their toroidal shape there exist regions of high and low magnetic field, so that the particles are divided into two classes - trapped ones that are periodically reflected in regions of high magnetic field with a characteristic frequency, and passing particles, whose parallel velocity is high enough that they largely follow a magnetic field line around the torus without being reflected. The radial drift that a particle experiences due to the field inhomogeneity depends strongly on its position, and the net drift therefore depends on the path taken by the particle. While the radial drift is close to zero for passing particles, trapped particles experience a finite radial net drift and are therefore lost in classical stellarators. These losses are described by the so-called neoclassical transport theory. Recent optimised stellarator geometries, however, in which the trapped particles precess around the torus poloidally and do not experience any net drift, promise to reduce the neoclassical transport down to the level of tokamaks. In these optimised stellarators, the neoclassical transport becomes small enough so that turbulent transport may limit the confinement instead. The turbulence is driven by small-scale-instabilities, which tap the free energy of density or temperature gradients in the plasma. Some of these instabilities are driven by the trapped particles and therefore depend strongly on the magnetic geometry, so the question arises how the optimisation affects the stability. In this thesis, collisionless electrostatic microinstabilities are studied both analytically and numerically. Magnetic configurations where the action integral of trapped-particle bounce motion, J, only depends on the radial position in the plasma and where its maximum is in the plasma centre, so-called maximum-J configurations, are of special interest. This condition can be achieved approximately in quasi-isodynamic stellarators, for example Wendelstein 7-X. In such configurations the precessional drift of the trapped particles is in the opposite direction from the direction of propagation of drift waves. Instabilities that are driven by the trapped particles usually rely on a resonance between these two frequencies. Here it is shown analytically by analysing the electrostatic energy transfer between the particles and the instability that, thanks to the absence of the resonance, a particle species draws energy from the mode if the frequency of the mode is well below the charateristic bounce frequency. Due to the low electron mass and the fast bounce motion, electrons are almost always found to be stabilising. Most of the trapped-particle instabilities are therefore predicted to be absent in maximum- J configurations in large parts of parameter space. Analytical theory thus predicts enhanced linear stability of trapped-particle modes in quasi-isodynamic stellarators compared with tokamaks. Moreover, since the electrons are expected to be stabilising, or at least less destabilising, for all instabilities whose frequency lies below the trapped-electron bounce frequency, other modes might benefit from the enhanced stability as well. In reality, however, stellarators are never perfectly quasi-isodynamic, and the question thus arises whether they still benefit from enhanced stability. Here the stability properties of Wendelstein 7-X and a more quasi-isodynamic configuration, QIPC, are investigated numerically and compared with another, non-quasiisodynamic stellarator, the National Compact Stellarator Experiment (NCSX) and a typical tokamak. In gyrokinetic simulations, performed with the gyrokinetic code GENE in the electrostatic and collisionless approximation, several microinstabilities, driven by the density as well as both ion and electron temperature gradients, are studied. Wendelstein 7-X and QIPC exhibit significantly reduced growth rates for all simulations that include kinetic electrons, and the latter are indeed found to be stabilising when the electrostatic energy transfer is analysed. In contrast, if only the ions are treated kinetically but the electrons are taken to be in thermodynamic equilibrium, no such stabilising effect is observed. These results suggest that imperfectly optimised stellarators can retain most of the stabilising properties predicted for perfect maximum-J configurations. Quasi-isodynamic stellarators, in addition to having reduced neoclassical transport, might therefore also show reduced turbulent transport, at least in certain regions of parameter space.
We present a Green's function based treatment of the effects of electron-phonon coupling on transport through a molecular quantum dot in the quantum limit. Thereby we combine an incomplete variational Lang-Firsov approach with a perturbative calculation of the electron-phonon self energy in the framework of generalised Matsubara Green functions and a Landauer-type transport description. Calculating the ground-state energy, the dot single-particle spectral function and the linear conductance at finite carrier density, we study the low-temperature transport properties of the vibrating quantum dot sandwiched between metallic leads in the whole electron-phonon coupling strength regime. We discuss corrections to the concept of an anti-adiabatic dot polaron and show how a deformable quantum dot can act as a molecular switch.
Synopsis
C+60 has been proposed to be responsible for two of the diffuse interstellar bands (DIBs), the absorption features observed in the visible-to-near-infrared spectra of the interstellar medium. However, a confirmation requires laboratory gas-phase spectra, which are so far not available. We plan to develop a novel spectroscopy technique that will allow us to obtain the first gas-phase spectra of C+60, and that will be applicable to other complex organic molecules such as polycyclic aromatic hydrocarbons. The current status of the experimental setup, the ideas behind the measurement scheme and the preparatory work toward its implementation will be presented.
Experience in the construction of optimized stellarators shows the coil system is a significant challenge. The precision necessary allow the generation of accurate flux surfaces in recent experiments affected both cost and schedule negatively. Moreover, recent experiments at Wendelstein 7-X have shown that small field corrections were necessary for the operation of specific desired magnetic configurations. Therefore, robust magnetic configurations in terms of coil geometry and assembly tolerances have a high potential to facilitate swifter and less expensive construction of future, optimized stellarators. We present a new coil optimization technique that is designed to seek out coil configurations that are resilient against 3D coil displacements. This stochastic version of stellarator coil optimization uses the sampling average approach to incorporate an iterative perturbation analysis into the optimization routine. The result is a robust magnetic configuration that simultaneously reproduces the target magnetic field more accurately and leads to a better fusion performing coil configuration.
A novel method for time-resolved tuned diode laser absorption spectroscopy has been developed. In this paper, we describe in detail developed electronic module that controls time-resolution of laser absorption spectroscopy system. The TTL signal triggering plasma pulse is used for generation of two signals: the first one triggers the fine tuning of laser wavelength and second one controls time-defined signal sampling from absorption detector. The described method and electronic system enable us to investigate temporal evolution of sputtered particles in technological low-temperature plasma systems. The pulsed DC planar magnetron sputtering system has been used to verify this method. The 2" in diameter titanium target was sputtered in pure argon atmosphere. The working pressure was held at 2 Pa. All the experiments were carried out for pulse ON time fixed at 100 (is. When changing OFF time the discharge has operated between High Power Impulse Magnetron Sputtering regime and pulsed DC magnetron regime. The effect of duty cycle variation results in decrease of titanium atom density during ON time while length of OFF time elongates. We believe that observed effect is connected with higher degree of ionization of sputtered particles. As previously reported by Bohlmark et al., the measured optical emission spectra in HiPIMS systems were dominated by emission from titanium ions [1].
Abstract
Reactive high power impulse magnetron sputtering (HiPIMS) of a cobalt cathode in pure argon gas and with different oxygen admixtures was investigated by time-resolved optical emission spectroscopy (OES) and time-integrated energy-resolved mass spectrometry. The HiPIMS discharge was operated with a bipolar pulsed power supply capable of providing a large negative voltage with a typical pulse width of 100 μs followed by a long positive pulse with a pulse width of about 350 μs. The HiPIMS plasma in pure argon is dominated by Co+ ions. With the addition of oxygen, O+ ions become the second most prominent positive ion species. OES reveals the presence of Ar I, Co I, O I, and Ar II emission lines. The transition from an Ar+ to a Co+ ion sputtering discharge is inferred from time-resolved OES. The enhanced intensity of excited Ar+* ions is explained by simultaneous excitation and ionisation induced by energetic secondary electrons from the cathode. The intensity of violet Ar I lines is drastically reduced during HiPIMS. Intensity of near-infrared Ar I lines resumes during the positive pulse indicating an additional heating mechanism.
Fluorocarbon containing capacitively coupled radio frequency (cc-rf) plasmas are widely used in technical applications and as model systems for fundamental investigations of complex plasmas. Absorption spectroscopy based on pulsed quantum cascade lasers (QCL) was applied in the mid-IR spectral range of 1269-1275 cm-1. Absolute densities of the precursor molecule CF4 and of the stable product C3F8 were measured with a time resolution of up to 1 ms in pulsed CF4/H2 asymmetrical cc-rf (13.56 MHz) discharges. For this purpose both the non-negligible temperature dependence of the absorption coefficients and the interference of the absorption features of CF4 and C3F8 had to be taken into account in the target spectral range. Therefore, at two different spectral positions composite absorption spectra were acquired under the same plasma conditions in order to discriminate between CF4 and C3F8 contributions. A total consumption of∼ 12 % was observed for CF4 during a 1 s plasma pulse, whereas C3F8 appeared to be produced mainly from amorphous fluorocarbon layers deposited at the reactor walls. A gas temperature increase by ∼ 100 K in the plasma pulse was estimated from the measurements. Additionally, not yet identified unresolved absorption (potentially from the excited CF4 molecule) was found during the àon-phase'.