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Because of the vital role of the liquid as interface in plasma medicine, this work is focused on the elucidation of the interaction of plasmas with biologically relevant liquids. The results of this thesis are an important step in the direction of the applications to real biological liquids such as blood and wound secretion ex vivo as well as in vivo. In this thesis the following questions are investigated and answered with the special focus on the free radicals as highly reactive and, therefore, hard to detect relevant group of chemical species: What is the impact of the atmospheric-pressure argon plasma jet on biologically relevant solutions? Which species are generated due to the plasma treatment of liquids? What is an appropriate detection procedure for the qualification and quantification of the short-lived species? Does the surrounding conditions influence the formation of liquid-phase reactive species and can this influence be used to tailor a desired liquid composition? What is the influence of the plasma surroundings? What is the influence of feed gas manipulation regarding the reactive species generation? Can these impacts be used for a selected reactive species composition generation? Does the treated liquid medium affect the plasma-generated reactive species output and in what way? Which are the underlying mechanisms and origins of the plasma-caused chemical changes in the solutions? Do reactive species exist, which origin is located in the gaseous phase? What is the impact of the plasma jet radiation?
Barrier corona (BC) arrangements are employed in different plasma-based applications such as material surface and exhaust gas treatments. However, a comprehensive study about the discharge behavior and properties in such strongly asymmetric arrangements is still missing. This dissertation is devoted to the detailed investigation of single microdischarges (MDs) in a sinusoidally driven BC discharge in air at atmospheric pressure. The discharge arrangement consist of a sharp metal pin and a dielectric-covered hemispherical electrode. It is the first study of volume BC discharges, in which phasially-resolved spatio-temporal development of the MDs are recorded using a multi-dimensional time-correlated single photon counting (TC-SPC) technique. The morphology of the MDs is recorded using an ICCD camera. A voltage probe and a current probe are employed to measure the applied voltage and current pulses. Furthermore, phase-resolved current measurements and statistical studies of current pulse amplitudes are realized using an oscilloscope.
Due to the asymmetric geometry and material of the electrodes, discharge behavior in the two polarities of the applied sinusoidal voltage is significantly different. For the voltage amplitude being applied, mostly two MDs appear in the anodic pin half-cycles. It is observed that the breakdown mechanism in both MDs is a positive streamer starting near the anode, similar to the single MDs in symmetric dielectric barrier discharges (DBDs). However, the second MDs have different properties, such as longer duration of the bulk plasma and broader current pulses. It is considered that the differences are mainly due to the positive surface charges deposited by the first MDs on the dielectric. It is proposed, for the first time, that the current pulse derivative maximum corresponds to the arrival of the streamer head at the cathode surface. This is used to synchronize the spatio-temporal development of the MDs with their current pulses. The accuracy of the synchronization is limited to the rise-time of the current probe (350 ps). In each cathodic pin half-cycle, only one major MD appears. The appearance and amplitude of the MDs are more erratic compared to the anodic pin polarity. The TC-SPC recordings show that the MDs appearing at low applied voltages have a similar spatio-temporal development to the MDs of the anodic pin polarity. On the other hand, at high applied voltages a development similar to transient sparks, i.e. a double-streamer starting near the tip of the pin (cathode), is observed. The statistical study shows that in DBD-like MDs the current pulse amplitude is not dependent on the appearance phase (or applied voltage), but this is not the case for the transient sparks.
Since BC reactors are also used for air cleaning, a set of experiments is done with 35 ppm toluene additive. It is observed that adding toluene results in 500~V lower breakdown voltage. Hence, the discharge in the presence of toluene is operated under over-voltage condition, resulting in stronger MDs in the anodic pin, and earlier-appearing as well as weaker MDs in the cathodic pin half-cycles.
The results of this dissertation about the spatio-temporal development and statistical behavior of the single MDs are foreseen to be employed in the study and optimization of plasma reactors, such as "Stacked DBD Reactor," which are developed for exhaust gas and material surface treatment. Furthermore, the results are a benchmark for the study of a novel discharge arrangement with a rotating dielectric electrode.
Organic molecules are the carbon-based complex of several atoms, is an innovative and essential element to create nano-structural platforms, as a building block in the
field of organic electronics and organic spintronics. Because of its variety and functionality via widely studied synthetic methods, molecules have played an important role in electronics as not only a transport channel in bulk form but also a tuning layer
at the interface of hetero structures. The potential of molecular layers has also stood out in spintronics, owing to its mass-low composition producing long spin life time.
Organic materials can be employed in spintronics applications, benefiting from their low cost, ease of processing, and chemical tunability. Beyond this advantage, the configuration
of molecules on a metal film displays unique phenomena as it can control the molecular spins and interfacial coupling between them, resulting in the emergence
of molecular spinterface.
This thesis work focuses on identifying the interfacial properties between the ferromagnet and the Phenalenyl (PLY) based metal complexes. The growth morphology study of the copper-phenalenyl Cu-PLY based molecules influence the electronic coupling between the molecular layer and the ferromagnet. Zinc- Phenalenyl (ZMP) molecule already have been studied [1] by demonstrate the formation of a spinterface,
resulting interface magneto resistance (IMR) close to room temperature. The
spinterface formation leads to the unique property, that a magnetic tunnel junction
with a ZMP barrier requires only one ferromagnetic metal layer, while the other ferromagnetic layer is formed in the organic barrier directly at the ferromagnet/organic
barrier interface. Here we compare Phenaleny, Copper-Phenaleny Cu-PLY and Zincmethyl- phenaleny molecule based MTJ electrical and magnetic properties which will
be suitable for tunnel barrier and can be used for stable memory devices. We tune the magnetic property of ferromagnet and forma hybrid interface without any oxide layers in between the ferromagnet and molecular layers. The tuning of magnetic properties
via the molecular approach will certainly extend versatile functionalities of organic spinterfaces.
The properties of the ion feature of the Thomson scattering signal are investigated. Firstly, the description of the atomic form factor by hydrogen-like wave functions is reviewed and better screening charges are obtained. Then the ionic structure in systems with several ion species is calculated from the HNC integral equation.
The importance of ion propulsion devices as an option for in-space propulsion of space
crafts and satellites continues to grow. They are more efficient than conventional chemi-
cal thrusters, which rely on burning their propellant, by ionizing the propellant gas in a
discharge channel and emitting the heavy ions at very high velocities. The ion emission
region of a thruster is called the plume and extends several meters axially and radially
downstream from the exit of a thruster. This region is particularly important for the effi-
ciency of a thruster, because it determines energy and angular distribution of the emitted
ions. It also determines the interaction with the carrier space craft by defining the electric
potential shape and the fluxes and energies of the emitted high energy ions, which are the
key parameters for sputter erosion of satellite components such as solar panels. Developing
new ion thrusters is expensive because of the high number of prototypes and testing cycles
required. Numerical modeling can help to reduce the costs in thruster development, but
the vastly differing length and time scales of the system, particularly the large differences of
scales between the discharge chamber and the plume, make a simulation challenging. Often
both regions are considered to be decoupled and are treated with different models to make
their simulation technically feasible. The coupling between channel and plume plasmas and
its influence on each other is disregarded, because there is no interaction between the two
regions. Therefore, this thesis investigates the physical effects which arise from this cou-
pling as well as models suitable for an integrated simulation of the whole coupled problem
of channel and plume plasmas. For this purpose the High Efficiency Multistage Plasma
Thruster (HEMP-T) ion thruster is considered.
For the discharge channel plasma, a fully kinetic model is required and the Particle-in-Cell
(PIC) method is applied. The PIC method requires very high spatial and temporal resolu-
tions which makes it computationally costly. As a result, only the discharge channel and the
near-field plume close to the channel exit can be simulated. In the channel, the results show
that electrons are magnetized and follow the magnetic field lines. The orientation of the
magnetic field there is mostly parallel to the symmetry axis and the channel walls which re-
sults in a high parallel electron transport and leads to a flat electric potential and a reduced
plasma-wall sheath. Only at the magnetic cusps, which are characteristic of HEMP-Ts the
electrons are guided towards the wall, with ions following due to quasineutrality, where a
classical plasma-wall sheath develops. The ion-wall contact is thus limited to the cusp re-
gion. The small radial drop of the potential towards the wall gives rather low energies of
ions impinging at the wall and minimizes erosion in the HEMP-T.
In the near-field plume, which extends from the thruster exit plane to some centimeters
downstream, the ion emission characteristics is defined. The ratio of radial and axial elec-
tric field components in this region determines the ion emission angle which should be
minimized for maximum thruster efficiency. The plasma discharge in the channel produces
high plasma densities and the subsequent drop from plasma to vacuum potential occurs
further downstream for higher densities. This increases the ratio of radial and axial electric
field components because the plasma expands radially outside of the confinement from the
dielectric discharge channel walls. The potential structure in the near-field plume impacts
also the supply of electrons for the channel discharge because the electrons enter the channel
from the plume. An effect which arises from this coupling is the breathing mode oscilla-
tion. It is an oscillation which is observed in all plasma quantities and is located near the
thruster exit. The oscillation frequency measured in the simulation is in good agreement
with a predator-prey estimate which validates this ansatz. However, the electron tempera-
ture, assumed constant in the predator-prey model, correlates inversely with the oscillation,
i.e. it is minimal at the current maximum and vice versa, which contributes to the observed
oscillations. Because of the oscillation of the plasma number density, the potential drop also
oscillates in the exit region and thus the ratio of radial to axial electric field components,
which results in the oscillation of the mean ion emission angle.
Regarding suitable models for a combined simulation of channel and plume plasmas, the
PIC model for channel and near-field plume is explicitly coupled to a hybrid fluid-PIC
model for the plume. The latter treats the electrons as a fluid, hence increasing the effective
spatial and temporal resolutions which can be applied in the plume simulations at the cost
of reduced accuracy of the electron model. Plasma densities decrease by two orders of
magnitude two meters downstream from the channel exit. The explicitly coupled kinetic
and hybrid PIC models are well suited for the computation of a HEMP-T and its plume
expansion, but they disregard the coupling of channel and plume plasmas for which other
methods are necessary. For this purpose a new approach is presented with a proof-of-
principle validation. The limited spatial resolution in the plume can be overcome with the
mesh-coarsening method, which increases the resolution in regions of low plasma density
without numerical artifacts. Sub-cycling for the electrons in the plume can then be used
to increase the temporal resolution in the plume. The combination of both methods, called
the sub-cycling mesh-coarsening (SMC) algorithm in the scope of this work, promises high
savings in computational cost which can make a combined simulation of plume and channel
plasmas feasible.
Particle and heat transport in fusion devices often exceed the neoclassical prediction. This anomalous transport is thought to be produced by turbulence caused by microinstabilities such as ion and electron-temperature-gradient (ITG/ETG) and trapped-electron-mode (TEM) instabilities, the latter ones known for being strongly influenced by collisions. Additionally, in stellarators, the neoclassical transport can be important in the core, and therefore investigation of the effects of collisions is an important field of study. Prior to this thesis, however, no gyrokinetic simulations retaining collisions had been performed in stellarator geometry. In this work, collisional effects were added to EUTERPE, a previously collisionless gyrokinetic code which utilizes the δ f method. To simulate the collisions, a pitch-angle scattering operator was employed, and its implementation was carried out following the methods proposed in [Takizuka & Abe 1977, Vernay Master's thesis 2008]. To test this implementation, the evolution of the distribution function in a homogeneous plasma was first simulated, where Legendre polynomials constitute eigenfunctions of the collision operator. Also, the solution of the Spitzer problem was reproduced for a cylinder and a tokamak. Both these tests showed that collisions were correctly implemented and that the code is suited for more complex simulations. As a next step, the code was used to calculate the neoclassical radial particle flux by neglecting any turbulent fluctuations in the distribution function and the electric field. Particle fluxes in the neoclassical analytical regimes were simulated for tokamak and stellarator (LHD) configurations. In addition to the comparison with analytical fluxes, a successful benchmark with the DKES code was presented for the tokamak case, which further validates the code for neoclassical simulations. In the final part of the work, the effects of collisions were investigated for slab and toroidal ITGs and TEMs in a tokamak configuration. The results show that collisions reduce the growth rate of slab ITGs in cylinder geometry, whereas they do not affect ITGs in a tokamak, which are mainly curvature-driven. However it is important to note that the pitch-angle scattering operator does not conserve momentum, which is most critical in the parallel direction. Therefore, the damping found in a cylinder could be the consequence of this missing feature and not a physical result [Dimits & Cohen 1994]. Nonetheless, the results are useful to determine whether the instability is mainly being driven by a slab or toroidal ITG mode. EUTERPE also has the feature of including kinetic electrons, which made simulations of TEMs with collisions possible. The combination of collisions and kinetic electrons made the numerical calculations extremely time-consuming, since the time step had to be small enough to resolve the fast electron motion. In contrast to the ITG results, it was observed that collisions are extremely important for TEMs in a tokamak, and in some special cases, depending on whether they were mainly driven by density or temperature gradients, collisions could even suppress the mode (in agreement with [Angioni et al. 2005, Connor et al. 2006]). In the case of stellarators it was found that ITGs are highly dependent on the device configuration. For LHD it was shown that collisions slightly reduce the growth rate of the instability, but for Wendelstein 7-X they do not affect it and the growth rate showed a similar trend with collisionality to that of the tokamak case. Collisions also tend to make the ballooning structure of the modes less pronounced.
In this thesis, I present work motivated, in part, by a series of upcoming laboratory experiments (APEX), which seeks to uncover some of the inner workings of turbulence and stability in electron- positron plasmas in closed field-line systems. I present the results of several distinct, but connected, problems addressing the theory of electron-positron plasmas.
This work is partitioned into several parts, which loosely correspond to different particulars of the APEX experiment and the different theoretical physics problems which reside within.
I begin with the derivation of a kinetic theory for plasmas which are optically thin to cyclotron emission, as indeed, experimental pair plasmas are expected to be. The results of this section include: (1) the derivation of a general kinetic theory of cyclotron radiation in electron-ion plasmas; (2) a calculation showing that cyclotron emission results in strongly anisotropic distribution functions on the radiation timescale; (3) calculation of the evolution of the distribution function under collisional scattering which, in the absence of any radiation terms, acts to drive the plasma towards a Maxwellian; (4) generalisation of this theory to more exotic geometries; (5) specialisation of this theory to pair plasmas of experimental interest; and (6) presentation of the applications and the limitations of this theory.
The second project is primarily concerned with non-neutral plasmas. We begin with gyrokinetic theory and a novel extension of this theoretical framework to plasmas with arbitrary degree of neutrality in straight field-line geometry. I go on to discuss the gyrokinetic stability theory of such plasmas in this simplified geometry. I conclude this project with a discussion of some further
nuances in the theory of singly-charged non-neutral plasmas, this time concerning global features. Namely, I declare an interest in the equilibria such plasmas might be able to attain.
The final project pertains to plasmas which are in state of Maxwellian equilibrium i.e., electron- positron plasmas with sufficiently large number densities of each species to attain a stationary quasineutral plasma. To this end, I present gyrokinetic flux-tube simulations of electron-positron plasmas in complex, and experimentally relevant, magnetic geometries on the road towards a study of gyrokinetic turbulence. The results of this work include: (1) the first simulations of electron- positron plasmas in a stellarator and ring-dipole geometry; (2) an analytic theory of trapped particle modes in electron-positron plasmas, a result which can also be verified numerically; and (3) extension of several important theoretical results in electron-positron plasmas to experimentally relevant geometries. The culmination of this project is the roadmap ahead towards demonstration of the so-called “inward pinch” effect in electron-positron plasmas in a magnetic Z-pinch.
This work examines the influence of monovalent and divalent cations on tetramyristoyl cardiolipin (TMCL) monolayers. A lipid monolayer can undergo an ordering transition of the lipid alkyl chains from a disordered fluid phase (liquid-expanded (LE)) to an ordered gel phase (liquid-condensed (LC)). Compression of the lipid monolayer in a Pockels-Langmuir trough was monitored with a Wilhelmy plate tensiometer, yielding the surface pressure π in dependence of the area a molecule can occupy on average A, as a π-A-isotherm. The onset of the first order LE/LC phase transition is marked by an abrupt change in the isotherm at surface pressure πc.
These associated lipid membrane changes were characterized by variation of the compression speed, kind and concentration of the monovalent and divalent salt, pH, and temperature. The CL monolayer phase transition was found to depend on the compression speed, yielding only a small variation in the compression isotherms.
For monovalent cations on the cardiolipin monolayer, the dependence on salt concentration of the lipid liquid gel phase transition surface pressure πc was determined and a non-monotonic behavior was found, with a maximum in πc for a salt concentration of 0.1 mol/l. The maximum in πc can be shifted with pH (e.g. pH = 4.2). This behavior extended to potassium, sodium and cesium cations in the subphase. No ion specific effects were observed, which pointed to the prevalence of electrostatic interactions in the system.
Different divalent salt subphases, of either magnesium, calcium, strontium, manganese, iron or zinc salts, with fixed sodium chloride concentration of 0.15 mol/l at pH of 5.8 and 25 °C were investigated. πc decreases upon addition of divalent salts to the subphase. This points to increased screening and binding effects. Strongest binding effects were observed for calcium and manganese cations.
The electrostatic interactions of the system were modeled with a mean-field theory: Grahame’s equation, and a simple law of mass action. CL is modeled at half its molecular area and half its charge, with a proton dissociation constant of the phosphate group Ka,intrinsic(PO4) = 0.1 mol/l. The agreement with the experiment was satisfactory.
A linear dependence of πc on the temperature was found for cardiolipin monolayers on all subphases. The isothermal area compressibility modulus KA is calculated from selected isotherms. It was found that the flexibility of the monolayer decreases with temperature and the area per molecule for the cardiolipin fluid phase.
The compression speed, monovalent salt concentration, pH, and selected divalent cations were investigated with the BAM. For all a sigmoidal growth of xgel with compression was observed. For high salt concentrations non-circular and dendritic domains were observed.
A simple model for the nucleation process was introduced, yielding an estimate of 20 nm for the critical domain radius, which is below the resolution of the BAM, but a common length scale in biological systems.
Low-pressure plasmas offer a unique possibility of confinement, control and
fine tailoring of particle properties. Hence, dusty plasmas have grown
into a vast field and new applications of plasma-processed dust particles
are emerging. There is demand for particles with special properties and
for particle-seeded composite materials. For example, the stability of
luminophore particles could be improved by coating with protective Al2O3
films which are deposited by a PECVD process using a metal-organic precursor gas.
Alternatively, the interaction between plasma and injected micro-disperse powder
particles can also be used as a diagnostic tool for the study of plasma surface
processes. Two examples will be provided: the interaction of micro-sized (SiO2)
grains confined in a radiofrequency plasma with an external ion beam as well as
the effect of a dc-magnetron discharge on confined particles during deposition
have been investigated.
This thesis is devoted to experiments on three-dimensional dust clouds which are confined in low temperature plasmas. Such ensembles of highly electrically charged micrometer-sized particles reveal fascinating physics, such as self-excited density waves and vortices. At the same time, these systems are challenging for experimental approaches due to their three-dimensional character. In this thesis, new optical diagnostics for dusty plasmas have been developed and, in combination with existing techniques, have been used to study these 3D dusty plasmas on different size and time scales.