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In this thesis, size-sensitive phenomena of three-dimensional dust crystals emerged in a low temperature plasma are presented. Depending on the number of particles in the system phase transitions, collective vortex motions and large-scaled expansions can be observed. To investigate these fascinating effects an advanced experimental setup as well as new evaluation methods have been developed. This thesis will present these new techniques and the gained insights.
Surface Stoichiometry and Depth Profile of Tix-CuyNz Thin Films Deposited by Magnetron Sputtering
(2021)
The laser-matter interaction is a topic of current research. In this context, the interaction of intensive laser radiation with atomic clusters is of special interest. Du to the small cluster size, the laser field can penetrate the whole cluster volume, which leads to a high absorption of energy in the cluster. As a result, plasmas with high density and high temperature are produced. In the early phase of the laser-cluster interaction, free electrons are initially created in the cluster due to tunnel ionization or photoionization. Via collisions of these electrons with the cluster atoms, the ionization is increased and thus a dense nanoplasma is produced, which is heated by the laser. If free electrons leave the cluster during the laser-cluster interaction (outer ionization), a positive charge buildup is created. The associated charge repulsion finally can lead to the fragmentation of the cluster due to Coulomb explosion. Experimentally, interesting phenomena emerging from laser-excited clusters are observed, e.g., the creation of fast electrons, the production of highly charged ions, and X-ray emission. In this dissertation, the interaction of Gaussian laser pulses in the infrared regime with argon and xenon clusters is simulated by means of a nanoplasma model. Considering laser intensities in the non-relativistic regime, the relevant processes such as ionization, heating and expansion are theoretically described in this model with a set of coupled rate equations and hydrodynamic equations. One focus of the thesis is on the heating of the nanoplasma via inverse bremsstrahlung (IB), which is due to the absorption of laser photons in electron-ion collisions. In particular, the important question is investigated whether the consideration of the ionic structure – that means, the nuclear charge and the bound electrons – modifies the electron-ion collisions and thus the IB heating rate. Starting from a quantum statistical description, effective electron-ion potentials are used which account for both the screening due to the dense plasma and the inner ionic structure. Within the quantum mechanical first Born approximation, the consideration of the ionic structure leads to a drastic increase of the IB heating rate, in particular for high nuclear charges and low ionic charge states. However, for the parameters relevant in experiments, the applicability of the first Born approximation is questionable. Therefore, quantum mechanical calculations going beyond the first-order perturbation theory are performed. In addition, the IB heating rate is investigated with different classical methods. These are based either on transport cross sections for elastic electron-ion scattering or on classical simulations of inelastic scattering processes. Also within the classical approaches, the consideration of the ionic structure leads to an increase of the heating rate. However, this increase is shown to be only moderate. In a further part, the thesis focuses on the question how the dynamics of the laser-cluster interaction is influenced by the consideration of excited states. This is explored exemplarily for argon clusters excited by single or double laser pulses. The consideration of excitation processes in the nanoplasma leads to a decrease of the electron temperature and to an increase of the density of free electrons. Moreover, it is shown that the consideration of excitation processes results in an essential acceleration of the ionization dynamics. As a consequence, the mean ionic charge state in the plasma as well as the number of highly charged ions is significantly increased. For the population of ground states and excited states within an ionic charge state Z, collisional deexcitation processes play an important role. By means of an analytical relation between excitation and deexcitation cross sections, the rates for the respective processes in the presence of the laser field are calculated. The role of deexcitation processes is studied in detail, showing that the inclusion of these processes is essential for the correct theoretical description of the photon emission from laser-excited clusters. Based on these results, the photon yield is calculated for selected radiative transitions resulting from highly charged argon ions in the UV and X-ray regime.
This work study a monolayer of branched poly(ethyleneimine (PEI) adsorbed onto oppositely charged surfaces with iron chelates or iron ions in the absorption solution. The conformation of adsorbed PEI is explored in the dependence of the composition of the adsorption solution by measuring the surface forces using atomic force microscopy (AFM) with the colloidal probe (CP) at different ionic strengths (INaCl) in surrounding aqueous solution. The surface coverage of these layers is investigated using X-ray reflectivity.
PEI solutions show different pH values with iron chelates (pH = 3), iron ions (pH = 4.67) or pure water (pH = 9.3) at room temperature. Low surface coverage of PEI at pH = 3 adjusted by monovalent ions was also observed. However, adsorbing PEI with iron ions or iron chelates and washing with pure water shifts the pH, leading to an adsorbed PEI layer with high coverage. In our observation, the influence of iron ions and iron chelates on the surface coverage of PEI film is stronger than the pH effect. PEI adsorbed from a pure water solution shows flat conformation. Surface force measurements with CP show that PEI adsorbed from solutions containing iron chelates or iron ions cause almost identical steric forces. The thickness of the brush L is determined as a function of the ionic INaCl in the measuring solution. It scales as a polyelectrolyte brush.
The maximum number density of gold nanoparticles (AuNPs) adsorbed onto the PEI brushes was identical and larger than on flatly adsorbed PEI. On the PEI layer with the larger surface coverage, the AuNPs aggregate; on the PEI layer with the lower surface coverage they do not aggregate. Taken together, these results contribute to understanding the mechanisms determining surface coverage and conformation of PEI and demonstrate the possibility of controlling surface properties, which is highly desirable for potential future applications.
In this thesis, we also investigate the top layer (PSS and PDADMA) of polyelectrolyte multilayer (PEM) films. PEM films were prepared by sequential adsorption of oppositely charged PEs on solid substrates. PEM films consist of polydiallyldimethylammonium (PDADMA) as polycation and the polystyrene sulfonate (PSS) as polyanion. PDADMA has a smaller linear charge density than PSS. For this system, two different growth regimes are known: parabolic and linear. I studied the top layer (PSS and PDADMA) conformation of PEM films and how the structure of this top layer is affected by increasing the number of PDADMA/PSS layer pairs N and the addition of salt to the surrounding solution.
The INaCl was changed during the force-distance measurements. PSS terminated films always show electrostatic forces at INaCl < 0.1 M and flat conformation. The surface charge density is always negative at INaCl < 0.1 M. The surface charge of the PSS top layer starts to turn from negative to positive at N ≥ 14. At N between 13 and 15, adsorbed PSS cannot compensate all the excess PDADMA charge. This leads to an accumulation of the positive extrinsic sites within the PSS terminated film beyond a specific N. At INaCl ≈ 0.1 M, an exponential decaying force was measured. This is an indication of unusual long-ranged hydration force (decay length λ-1 ≈ 0.2-0.5 nm), and PSS terminated film shows zwitterionic or neutral surface. At INaCl > 0.1 M, a non-electrostatic action occurs and the PSS terminated film reswells in solution.
PDADMA terminated surface consisting of few layers show a flat conformation and the electrostatic forces were measured. For N ≥ 9 and INaCl ≤ 0.1 M, steric forces were measured. The force-distance profiles are well-explained by Alexander and de Gennes theory. PDADMA chains show a maximum L that is around 40-45 % of the contour length. For INaCl ≈ 0.1 M, and N > 9, a flat, neutral or zwitterionic surface is found (λ-1 ≈ 0.3-0.9 nm). For N = 9 and INaCl > 0.1 M, a strong screening of electrostatic interaction and attractive forces are observed. For N > 9 and INaCl > 0.1 M, the ion adsorption into the PE chains leads to an increase in the monomer size and as a result, the L increases and PDADMA brushes reswell again into the solution.
These data show that by varying N and INaCl, different surface forces can be obtained: Electrostatic forces (flat chains) both positive and negative, steric forces (brush), hydration force (flat, neutral or zwitterionic surface), and effects not yet explained (reswelling brush).
Synopsis
A network of ion sources is being developed on the 300-kV acceleration platform of the cryogenic storage ring (CSR) at the Max-Planck-Institut für Kernphysik. It consists of several types of sources like a metal ion sputtering source (MISS), a Penning source, a laser vaporization (LVAP) source, and an electrospray ionization (ESI) source to produce a large variety of ions which can be studied for photon and electron interaction in a ro-vibrationally cold environment. Furthermore a storage device such as a radiofrequency quadrupole (RFQ) is foreseen for internal state cooling and accumulation of rarely produced species.
The main objective of this work is to contribute to the understanding of the grafting of nitrogen and amino surface functional groups on polymers by means of plasmas containing nitrogen and hydrogen. For this purpose, many aspects of plasma surface modification were studied. In the frame of this work, a new, UHV-sealed plasma reactor system was put into operation. The system is special for its clean reaction environment and the possibility to perform quasi in situ XPS measurements. A comparison of the UHV system to a fine vacuum reactor showed that a clean reaction environment is mandatory for reproducible plasma processing and efficient nitrogen and amino functionalisation. A key motivation for the present work was the observation that the non-coating plasma processes reported in literature fail to graft primary amino groups on polymer surfaces with densities that significantly exceed 3 - 4% NH2/C. In order to investigate this phenomenon in detail, this work followed two experimental tracks: On the one hand, a broad systematic study of plasma processing parameters was performed. On the other, the surface diagnostics methods used for the quantification of amino groups were critically reviewed. For this, a numerical algorithm was developed to reconstruct the element depth profile from angle-resolved XPS data. In the scope of the process parameter study, cw and pulsed microwave (MW) plasma excitation was compared to radio-frequency (RF) excitation. The home-built MW source was studied and optimised with respect to ignition behaviour and power efficiency. The performance of the MW and RF plasmas in polymer surface modifications was studied in various gas mixtures containing NH3 and H,, or N2 and H,. Also the differences of glow and afterglow processing of polymers were investigated. Large variations of the nitrogen and primary amino grafting efficiencies were obtained. They triggered a number of new ideas for the underlying reaction mechanisms. Special attendance was devoted to the selectivity of the functionalisation processes for primary amino groups. Nitrogen-containing discharges that were rich in hydrogen achieved selectivities up to 100%. The upper limit of 3 - 4% amino groups on the surface, however, was not passed. Angle-resolved XPS measurements revealed a systematic problem for the definition of a surface density, which is capable of explaining the upper limit for amino groups. It is either due to a limited labelling depth of amino groups by the applied TFBA derivatisation reaction, or to a limited functionalisation depth of the plasma process. One very efficient nitrogen-grafting plasma process that was developed on polystyrene was applied to seven other unfluorinated polymers. The similarity of the resulting functionalisation demonstrated a good transfer-ability of plasma surface functionalisation processes. Plasma treatments of polymer surfaces, especially in hydrogen-containing gases, are known to be generally followed by uncontrollable oxidation phenomena. The properties of plasma-functionalised polymer surfaces were therefore studied in conjunction with ageing effects. Quasi in situ XPS analysis allowed to distinguish the influence of oxygen contamination during the plasma process from post-process oxidation due to contact of plasma-treated samples to atmospheric oxygen. The surface modification experiments were accompanied by several gas phase diagnostic techniques. In the scope of this work, the UHV reactor system was equipped with optical emission spectroscopy (OES), two-photon absorption laser-induced fluorescence (TALIF), and tunable diode laser absorption spectroscopy (TDLAS). A separate plasma source was setup to perform an absolute quantification of the vacuum-ultra-violet (VUV) emission intensity of hydrogen-containing MW-excited plasmas. The techniques were evaluated with respect to their contribution to an understanding of the plasma processing of polymers. The rich experimental data allowed to suggest new reaction mechanisms for the grafting of nitrogen- and amino functional groups. Surface passivation experiments in H, plasmas of nitrogen-functionalised surfaces initiated a re-evaluation and an extension of the mechanism of selective etching [1]. Together with two other new reaction mechanisms, a hypothetical reaction scheme was suggested. It was studied by the help of two numerical models for heterogenous reactions of radicals with the surface. In order to avoid the complexity of the fragmentation process of NH,, the models were restricted to discharges in N, and H9. Despite the sparse information on the composition of the gas phase, the data of two experimental series showed a very particular phenomenology that allowed a first test of the model. The test supports the newly-suggested reaction mechanisms. Especially the role of NH2 attachment to open reaction sites for the grafting of amino groups was emphasised. A more stringent test of the model is left to future experiments with extended gas phase diagnostic means.
In this thesis, the transport properties of topological insulators are investigated. In contrast to trivial insulators, topological insulators possess conducting boundary states which cross the bulk energy gap that separates the highest occupied electronic band from the lowest unoccupied band. The materials used in this thesis are three-dimensional topological insulators with time-reversal symmetry. Their associated helical surface states are protected against elastic backscattering by Kramers degeneracy. The unique properties of the helical surface states can be utilized to generate spin-polarized currents at the surface of topological insulators and to control their propagation direction. This makes them a promising material class for the field of spintronics.
Here, we perform photocurrent scans of topological insulator Hall bar and nanowire devices. From these measurements, we obtained two-dimensional maps of the polarization-independent and helicity-dependent components of the photocurrents.
We find that the polarization-independent component is dominated by the Seebeck effect and thus driven by thermoelectric currents. On the other hand, the helicity-dependent component is driven by the spin-polarized currents that emerge from the topologically non-trivial helical surface states via the circular photogalvanic effect.
First and foremost, our experiments demonstrate that topological insulator nanowires provide a promising platform for the generation of spin-polarized currents, whose direction can be controlled via the helicity of the excitation light. They also highlight the importance of analysing the spatial distribution of the photocurrent, as we observe a strong enhancement of the spin-polarized current and the thermoelectric current at the interface between the nanowire and the metallic contacts. As our analysis shows, the thermoelectric current is enhanced by the Schottky effect and the spin-polarized current is amplified by the spin Nernst effect. In addition, the spin Nernst effect is also present in Hall bar devices and manifest as an enhancement of the spin-polarized current along the Hall bar sides.
The extraction of raw materials in mining, as for example copper, generally requires a separation of the natural resources quarried. In most cases complex ores, mixtures of different minerals and gangue have to be separated in order to enable an economic processing. In particular for the extraction of sulfides, oxides, carbonates, phosphates, but also of coal, froth flotation is mainly used for this purpose, therefore it is considered as the most important separation process in raw material industries. Several billion tons of ores are processed annually. The principle of flotation is based on the surface properties of the mixtures components and the separation efficiency, which decisively determines the required amount of water and various chemicals, if nothing else, is an important criterion in mineral exploration and it also significantly influences the environmental impact of mineral processing. The aim of, this work was to investigate the influence, of, low-temperature plasmas on the mineral surface and, based on the acquired knowledge, to develop and verify strategies that would increase the efficiency of flotation processes through plasma pre-treatment of mineral mixtures. Since these studies are unprecedented, the results presented can be classified as a contribution to application-oriented basic research. Powder of the sulfide minerals, pyrite (FeS2), chalcopyrite (CuFeS2), chalcocite (Cu2S) and molybdenum sulfide (MoS2), were treated with plasmas of a radiofrequency and a microwave discharge and the resulting surface modifications were investigated by structure analysis such as X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD). During the plasma process, the argon/oxygen and argon/hydrogen process gas mixtures used were analyzed by mass spectrometry (MS), taking into account the quantity of gaseous reaction products released, in order to estimate the rate at which chemical reactions occur. Furthermore, Langmuir and thermal probes, as well as different methods of optical emission spectrometry (OES) were utilized, which enabled a characterization of the discharges used with regard to different plasma parameters. It has been shown that sulfur dioxide (SO2) in Ar/O2 plasmas and hydrogen sulfide (H2S) in Ar/H2 plasmas are the only reaction products which can be detected by MS during the mineral treatments. Thus, the resulting sulfur rate loss could be time-resolved determined by means of additional calibrations with calibrating gases. Especially at Ar/O2-MW plasma treatments two fundamental mechanisms of mineral modification could be separated by time. Pure plasma-surface interactions at the beginning and, additionally, thermally induced reactions in during the evolution of the treatments. Comparisons regarding the relative sulfur loss during plasma-surface interactions between the investigated minerals have shown a strong influence of the process parameters whereas, under identical conditions, CuFeS2 reacted up to eight and nineteen times faster reacted than FeS2 or Cu2S. This result represents the basis of the strategy to optimize the flotation of the minerals investigated: The selective generation of oxides on the surface of one component in a mixture of sulphide minerals. In particular, at the separation of CuFeS2/FeS2 mixtures by using the oxide collectors Flotinor Fs-2 in a micro flotation cell, a high selectivity could be achieved. The recovery of CuFeS2 amounted to 100 % while less than 10 % of FeS2 was recovered and no other modifying reagents were used. XPS and XRD analyses indicate the possibility that metal oxide are created upon the CuFeS2 surface, while the formation of iron sulfates upon the FeS2 surface prevented the oxide collector adsorption. An increased intensity of the plasma treatment leads to an increased sulphate formation also on CuFeS2, whereas the recovery, and thus the selectivity of the flotation, was reduced again. It could be shown that this effect can be utilized for the separation of, CuFeS2/MoS2 mixtures by using both, oxide and sulfide collectors, because sulfates are not formed on molybdenum sulfide during Ar/O2 plasmas treatments. By means of the plasma diagnostics used the energy input onto the substrate, the gas temperature and the degree of dissociation of molecular gases were estimated and correlations regarding the surface modification have been worked out. Thereby, the region investigated within the parameter space could be enlarged due to the use of different excitation frequencies, 13.56 MHz and 2.45 GHz, and additional insights have been provided. Further studies, beyond the scope of this work, are, nevertheless, required in order to generate a more comprehensive picture of plasma-mineral interactions and to enable an optimal application of the obtained results.
Abstract
To suit a wide variety of space mission profiles, different designs of ion thrusters were developed, such as the High‐Efficiency‐Multistage‐Plasma thrusters (HEMP‐T). In the past, the optimization of ion thrusters was a difficult and time‐consuming process and evolved experimentally. Because the construction of new designs is expensive, cheaper methods for optimization were sought‐after. Computer‐based simulations are a cheap and useful method towards predictive modelling. The physics in HEMP‐T requires a kinetic model. The Particle‐in‐Cell (PIC) method delivers self‐consistent solutions for the plasmas of ion thrusters, but it is limited by the high amount of computing time required to study a specific system. Therefore, it is not suited to explore a wide operational and design space. An approach to decrease computing time is self‐similarity scaling schemes, which can be derived from the kinetic equations. One specific self‐similarity scheme is investigated quantitatively in this work for selected HEMP‐Ts, using PIC simulations. The possible application of the scaling is explained and the limits of this approach are derived.
Modern space missions depend more and more on electric propulsion devices for in-space
flights. The superior efficiency by ionizing the feedgas and propelling them using electric
fields with regard to conventional chemical thrusters makes them a great alternative. To
find optimized thruster designs is of high importance for industrial applications. Building
new prototypes is very expensive and takes a lot of time. A cheaper alternative is to rely
on computer simulations to get a deeper understanding of the underlying physics. In order
to gain a realistic simulation the whole system has to be taken into account including the
channel and the plume region. Because numerical models have to resolve the smallest time
and spatial scales, simulations take up an unfeasible amount of time. Usually a self-similarity
scaling scheme is used to greatly speed up these simulations. Until now the limits of this
method have not been thoroughly discussed. Therefore, this thesis investigates the limits
and the influence of the self-similarity scheme on simulations of ion thrusters. The aim
is to validate the self-similarity scaling and to look for application oriented tools to use
for thruster design optimization. As a test system the High-Efficiency-Multistage-Plasma
thruster (HEMP-T) is considered.
To simulate the HEMP-T a fully kinetic method is necessary. For low-temperature plasmas,
as found in the HEMP-T, the Particle-in-Cell (PIC) method has proven to be the best
choice. Unfortunately, PIC requires high spatial and temporal resolution and is hence
computationally costly. This limits the size of the devices PIC is able to simulate as well
as limiting the exploration of a wider design space of different thrusters. The whole system
is physically described using the Boltzmann and Maxwell equations. Using these system
of equations invariants can be derived. In the past, these invariants were used to derive a
self-similarity scaling law, maintaining the exact solution for the plasma volume, which is
applicable to ion thrusters and other plasmas. With the aid of the self-similarity scaling
scheme the computation cost can be reduced drastically. The drawback of the geometrical
scaling of the system is, that the plasma density and therefore the Debye length does not
scale. This expands the length at which charge separation occurs in respect to the system
size. In this thesis the limits of this scaling are investigated and the influence of the scaling
at higher scaling factors is studied. The specific HEMP-T design chosen for these studies is
the DP1.
Because the application of scaling laws is limited by the increasing influence of charge separation with increased scaling, PIC simulations still are computationally costly. Another approach to explore a wider design space is given using Multi-Objective-Design-Optimization
(MDO). MDO uses different tools to generate optimized thruster designs in a comparatively
short amount of time. This new approach is validated using the PIC method. During this
validation the drawback of the MDO surfaces. The MDO calculations are not self-consistent
and are based on empirical values of old thruster designs as input parameters, which not
necessarily match the new optimized thruster design. By simulating the optimized thruster
design with PIC and recalculate the former input parameters, a more realistic thruster design is achieved. This process can be repeated iteratively. The combination of self-consistent
PIC simulations with the performance of MDO is a great way to generate optimized thruster
designs in a comparatively short amount of time. The proof of concept of such a combination
is the pinnacle of this thesis.