Insight into the relationship between the Ionization Energy (IE) offsets between donor and acceptor materials and the performance of the organic solar cells (OSC) could improve the charge generation efficiency. Charge generation can proceed through two different paths in Bulk Heterojunction (BHJ) based OSCs which are electron transfer from donor to acceptor and hole transfer from acceptor to donor. Electron transfer can be controlled by electron affinities and hole transfer can be controlled by ionization energies. In this work, large IE offsets were investigated in poly(3-hexylthiophene-2,5-diyl)(P3HT):Non Fullerene Acceptor (NFA) based OSCs by fabricating and characterizing devices, also conducting several experiments to optimize the processing conditions for the devices. These results provide an overview of the charge transfer and IE offsets dependence, also a general picture of the photophysics in P3HT:NFAs based OSCs. Moreover, using wide bandgap polymer donor which has shallow IE such as P3HT with low-bandgap NFAs may provide sufficient IE offsets between donor and acceptors enabled us to reach the inverted Marcus regime. In this regime, the electron transfer rate decreases upon decreasing the charge transfer (CT) state energy compared to the exciton energy. The decrease of the internal quantum efficiency (IQE) upon increasing the IE offset suggests that we are in that regime.

The introduction of ionization under ambient conditions has greatly simplified mass spectrometric analysis. Over past decade, ambient ionization mass spectrometry (MS) methods have revolutionized the way complex samples are analyzed under environmental conditions without requiring, in most cases, any sample pretreatment. Ambient ionization MS gained popularity among other analytical techniques due to its simplicity and its suitability for analysis of small and large molecules. However, ambient ionization methods can suffer from low accuracy and sensitivity due to matrix effects and interferences within complex samples, as well as from poor ionization efficiency. Matrix effects in ambient ionization are usually caused by ion suppression and may depend on different factors, e.g. matrix-to-analyte concentration ratios, proton affinities of analyte and matrix species. To overcome these challenges, in this thesis we present a new approach where a probe is used both as a direct sampling device and as an efficient ambient ionization source. This approach leverages high surface area gold electrodes, fabricated through low-cost bench-top fabrication methods and functionalized using self-assembled alkyl thiol monolayers, as functional conductive sampling probes (FCSPs) for the extraction and concentration of analytes from a sample solution. FCSPs loaded with the targeted analytes were then used to demonstrate a new and highly efficient ionization approach, called Primary Ion Mass Spectrometry Source (PIMSS). In this approach, following capture, the bound analytes are directly desorbed into the mass spectrometer, where ionization is achieved solely through the extraction voltage applied to the probe. 3D-printing was used to design an interface to couple FCSPs to the mass spectrometer. In this work, we discuss a detailed method development and optimization stage and present capabilities of the proposed assay. / Thesis / Master of Science (MSc)

A new semi-empirical model is introduced for the quantification of inductively-coupled breakdown systems. The model is informed by breakdown studies conducted on the Modular Theta-pinch eXperiment (MTX). Observations made of inductively-coupled breakdown behaviour are consistent with the model's expectations, indicating that the model can be used to aid in design of inductively-coupled pre-ionization systems. The model is further found to be capable of quantifying the efficacy of seed ionization in inductively-coupled systems. Comparisons are made between the standard ringing-theta and a new field-aligned dipole pre-ionization systems. In the presence of sufficient seed ionization, no physical reason was observed for selection of one method over the other, leaving only engineering considerations as the determining factor for selection of an appropriate pre-ionization system. This work is supported by the Institute for Critical Technology and Applied Science (ICTAS) at Virginia Tech and the National Nuclear Security Administration of the U.S. Department of Energy. LA-UR-24-31269 / Doctor of Philosophy / A new experiment at Los Alamos National Laboratory called the Modular Theta-pinch eXperiment (MTX) has been constructed to explore a variety of applications of Field-Reversed-Configurations (FRCs). An FRC is a plasma torus with a unique magnetic field configuration that has potential applications for astrophysical shock studies, fusion energy, and space proplusion. The first step in forming an FRC is the pre-ionization step, in which a plasma is created with a magnetic field diffused throughout its volume. The first purpose of this study is to better characterize inductively-coupled breakdown. Breakdown refers to the transition of a gas into a plasma (the fourth state of matter). To do this using inductively-coupled methods means that oscillating magnetic fields are used to induce electric fields in the gas, which cause electrons to gain energy and eventually collide with gas particles, creating a plasma. The second purpose of this study is to compare the more common ringing-theta pre-ionization method to a field-aligned method. Ringing-theta systems have been observed to encounter difficulties with diffusion of magnetic field into the pre-ionized plasma and field-aligned methods are a potential alternative that can circumvent the problems that ringing-theta systems encounter. Together, these studies should allow for other experimentalists to more easily design pre-ionization systems for both FRC experiments and general plasma physics experiments.

A new era of high-throughput mass spectrometry emerged with the nearly simultaneous introduction of two ambient ionization techniques: desorption electrospray ionization (DESI) and direct analysis in real time (DART). The ability to integrate near instantaneous sample analysis with the specificity of mass spectrometry opened up a broad range of applications. While some of these involve the direct analysis of bulk materials, many others require the collection and deposition of samples onto suitable substrates. This dissertation details the development of a new mode of operation for DESI. Instead of depositing a sample onto a continuous surface, the sample is either collected by or deposited onto a mesh substrate. Analytes either adsorb to the mesh strands or become suspended within the confines of the mesh in macroscale droplets. The samples are then analyzed by scrolling the mesh orthogonally into the path of an electrospray plume positioned coaxial to the inlet capillary of the mass spectrometer, thereby resulting in the transmission of the ionizing plume directly through the material. The transmission mode results in desorption and ionization typical of DESI, but with the added benefits of a simpler experimental geometry and the convenient analysis of both dry (i.e., following evaporation of the deposition solvent) and wet (i.e., solvated) samples. The simplification of the experimental arrangement increases method robustness and reproducibility, while the inclusion of a mesh substrate introduces new possibilities for sample collection and introduction, due to the intricate chemistry between the mesh material, analytes, and deposition/electrospray solvent system. However, the most important benefit lies in the development of surface-enhanced TM-DESI, whereby mesh substrates are derivatized to specifically capture and concentrate targeted analytes directly from solution. Following removal of matrix interferences by sample rinsing and subsequent cleavage of a photolabile linker, the mesh is analyzed directly by TM-DESI-MS. The technique has the potential to overcome interferences that have typically required chromatographic separations using LC-MS or have been insurmountable using ambient ionization methods. The impact of the surface-enhanced method could be tremendous as it may ultimately unite the competing metrics of analytical speed and specificity for ambient ionization mass spectrometry. / text

The dissociative ionization by electron impact of H₂, H₂O, and H₂S was investigated between the electron impact energies of 20 and 45 eV. Protons were the detected fragments, and a time-of-flight method was used to measure the proton kinetic energies. By also measuring the thresholds for the production of discrete energy groups of protons, it was possible to determine the dissociation limits and kinetic energy distributions for individual electronic states. It was found that autoionizing states that lead to dissociation were the major contributors of proton fragments for all of the molecules investigated. Some of the measurements are tabulated in the following table. (UNFORMATTED TABLE FOLLOWS) Molecule Threshold Dissociation Probable Probable (eV) limit (eV) state fragments H₂ 24.5±1.0 18.0±1.0 Q₁ ¹Σ(g)⁺ H⁺, H(1S) 30.5±1.0 18.0±1.0 Q₁ ¹Πᵤ H⁺, H(1S) 36.5±1.0 -- ²Πᵤ H⁺, H(2P) H₂O 24.5±1.0 19.5±1.0 -- H⁺, OH (X²Π) 29.5±1.0 23.0±1.0 -- H⁺,O(³P),H(1S) H₂S 25.5±1.0 18.0±1.0 -- H⁺, HS (X²Π) 32.0±1.0 -- -- H⁺, . . . 42.0±1.0 -- -- H⁺, . . . (TABLE ENDS)

A dissertation submitted to the Faculty of Science, University of Witwatersrand, Johannesburg, in fulfilment of the requirements for the degree of Master of Science. / In this dissertation a recipe has been outlined on how thrust can be calculated using the conservation of momentum in continuum form. With the aim of modelling a CORION (corona ionization) like thruster in mind it was then argued using a much simpler system and stochastic calculus why a statistical description of the system is necessary. From this the one-particle distribution emerged as a natural tool for the description of a system su cient for the determination of the system's thrust.This was followed by a short investigation into the background of non-equilibrium statistical mechanics, both classical and quantum, necessary to understand how one-particle distributions could be derived formally and in a physically consistent way. Mass ow and current-voltage experiments of the CORION like thrust system, necessary for characterization of part of the system, were conducted. This led to a proposal for a modelling strategy, consisting of merging di erent modelling approaches and descriptions considered throughout the dissertation.

Thesis (M.Sc.)--York University, 2007. Graduate Programme in Chemistry. / Typescript. Includes bibliographical references (leaves 71-75). Also available on the Internet. MODE OF ACCESS via web browser by entering the following URL: http://gateway.proquest.com/openurl?url_ver=Z39.88-2004&res_dat=xri:pqdiss&rft_val_fmt=info:ofi/fmt:kev:mtx:dissertation&rft_dat=xri:pqdiss:MR38780

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