During my master thesis I became familiar with ion imaging and velocity map imaging (VMI) techniques in experiments with molecular beam. My major contribution was writing a computer program for data acquisition and pre-analysis. The program features initial filtering of the data, improving significantly signal to noise ratio. Non-trivial effort was required to make the program compatible with three different CCD cameras implemented on different experiments in the laboratory. I have also simulated ion trajectories in VMI and wrote a program code to imulate VMI image distortions due to imperfections in apparatus geometry. These programs will be useful in aligning and tuning the apparatus. Finally, I wrote a program for data manipulation and conversion to formats compatible with various data analysis programs available in the laboratory. All the above programs I have tested by measurements of 243 nm photodissociation of HBr molecules.

No description available.

Detailed investigations of molecular collisions at the gas-surface interface provide insight into the dynamics and mechanisms of important interfacial reactions. A thorough understanding of the fundamental interactions between a gas and surface is crucial to the study of heterogeneous chemistry of atmospheric organic aerosols. In addition to changing the chemical and physical properties of the particle, reactions with oxidizing gases may alter aerosol optical properties, with implications for the regional radiation budget and climate. Molecular beams of CO₂, NO₂ and O₃ were scattered from long-chain methyl (CH₃-), hydroxyl (OH-), vinyl (H₂C=CH-) and perfluorinated (CF₃(CF₂)₈-, or F-) ω-functionalized alkanethiol self-assembled monolayers (SAMs) on gold, to explore the reaction dynamics of atmospherically important triatomics on proxies for organic aerosols. Energy exchange and thermal accommodation during the gas-surface collision, the first step of most interfacial reactions, was probed by time-of-flight techniques. The final energy distribution of the scattered molecules was measured under specular scattering conditions (θi = θf = 30°). Overall, extent of energy transfer and accommodation was found to depend on the terminal functional group of the SAM, incident energy of the triatomics, and gas-surface intermolecular forces. Reaction dynamics studies of O3 scattering from H2C=CH-SAMs revealed that oxidation of the double bond depend significantly on O₃ translational energy. Our results indicate that the room-temperature reaction follows the Langmuir-Hinshelwood mechanism, requiring accommodation prior to reaction. The measurements also show that the dynamics transition to a direct reaction for higher translational energies. Possible environmental impacts of heterogeneous reactions were probed by evaluating the change in the optical properties of laboratory-generated benzo[a]pyrene (BaP)-coated aerosols, after exposure to NO₃ and NO₂, at 532 nm and 355 nm by three aerosol analysis techniques: cavity ring-down aerosol spectroscopy (CRD-AS) at 355 nm and 532 nm, photoacoustic spectroscopy (PAS) at 532 nm, and an aerosol mass spectrometer (AMS). Heterogeneous reactions may lead to the nitration of organic-coated aerosols, which may account for atmospheric absorbance over urban areas. Developing a detailed understanding of heterogeneous reactions on atmospheric organic aerosols will help researchers to predict the fate, lifetime, and environmental impact of atmospherically important triatomics and the particles with which they collide. / Ph. D.

No description available.

<p>  </p> <p>Research that seeks to understand and develop the growth of III-nitride materials by molecular beam epitaxy (MBE) is beneficial to a broad range of the device community. MBE and the III-nitrides have been used to develop transistors, diodes, electroacoustic devices, solar cells, LEDs, LDs, intersubband devices, and quantum-cascade lasers. In this work we focus on the growth of III-nitride materials specifically for applications in near-infrared intersubband (NIR ISB) optical devices, however all this work is broadly applicable. </p> <p><br></p> <p>We begin by investigating the reduced indium incorporation in non-polar m-plane InGaN films. We find that InGaN grown on m-plane GaN has an effective activation energy for thermal decomposition of 1 eV, nearly half that reported for similar c-plane films. We produce high quality m-plane In0.16Ga0.84N and utilize it in AlGaN/InGaN devices designed for near-infrared ISB absorption measurements. We continue this work by exploring the growth of low-temperature AlGaN, necessary for these devices. We find that the utilization of an indium surfactant during low-temperature AlGaN growth enhances adatom diffusion, resulting in smoother surface morphologies, sharper interfaces, and reduced defects within the material. This growth method also prevents the anomalous suppression of the AlGaN growth rate, which we link to a reduction in the formation of high-aluminum containing defects. These investigations result in the demonstration of an Al0.24Ga0.76N/In0.16Ga0.84N heterostructure with a conduction band offset large enough to enable NIR ISB transitions.</p> <p><br></p> <p>Lastly, we explore the novel material ScAlN. This material’s large bandgap, large spontaneous polarization, ferroelectricity, and ability to be lattice matched to GaN at ~18% scandium composition make it an ideal candidate for a variety of devices, including NIR ISB devices. We investigate the reported temperature dependence of ScAlN’s <em>c</em>-lattice constant and confirm this dependence is present for high growth-temperature ScxAl1-xN with 0.11 < x < 0.23. We find that this temperature dependence is no longer present below a certain composition-dependent growth temperature. This finding, coupled with observations that samples grown at lower temperatures exhibit lower defect densities, smoother surfaces, and homogeneous chemical compositions suggest that high growth temperatures lead to defect generation that may cause the observed change in lattice parameters. We demonstrate lattice-matched, 50 repeat Sc0.18Al1-xN/GaN heterostructures with ISB absorption in excess of 500 meV with FWHM as little as 45 meV. </p>

No description available.

Das Wachstum von monolagen dünnen Schichten von InN und GaN/InN auf ZnO wurde untersucht. Ebenso der Einfluss der Verspannung, welche durch das Substrat bedingt ist, auf den Indiumgehalt von (In, Ga)N Heterostrukturen, welche auf GaN und ZnO gewachsen wurden. Alle Proben wurden mittels Molekularstrahlepitaxy gewachsen. Es wurde eine Prozedur entwickelt zum Glühen von ZnO Substraten, um glatte Oberflächen mit Stufenfluss-Morphologie zu erhalten, welche sich für das Wachstum von monolage-dünnen Heterostrukturen eignen. Solche Zn-ZnO und O-ZnO Oberflächen konnten produziert werden, wenn die Proben bei 1050 °C in einer O2 Atmosphäre bei 1 bar für eine Stunde geglüht wurden. Reflection high energy electron diffraction wurde eingesetzt, um in situ den Wachstumsmodus und die Entwicklung des a-Gitterabstandes zu untersuchen. Die kritische Schichtdicke, ab welcher ein Übergang im Wachstumsmodus von glattem zu rauhem Wachstum statt findet, war für das Wachstum von InN auf ZnO geringer als 2 ML und setzt gemeinsam mit dem Beginn der Relaxation ein. Für das Wachstum von GaN auf monolagen-dünnem InN/ZnO konnte gezeigt werden, dass höchstens wenige ML abgeschieden werden können, bevor Relaxation eintritt und/oder eine Vermischung zu (In, Ga)N stattfindet. Untersuchungen durch Röntgenbeugung und Raman Spektroskopie geben Hinweise darauf, dass das Abscheidung der nominalen Struktur 100x(1 ML InN/2 MLs GaN) vermutlich zum Wachstum von (In, Ga)N führte. Die chemische Zusammensetzung war für alle Proben sehr ähnlich mit einem indium Gehält von etwa x: 0.36 und einem Relaxationsgrad von 65% - 73% für Proben, die auf ZnO gewachsen wurde und 95% für Wachstum auf 300 nm In0.19Ga0.81N/GaN. Ein unbeabsichtigter Unterschied im V/III-Verhältnis während des Wachstums von (In, Ga)N Heterostrukturen, auf welchen die Anwesenheit von Metalltröpchen auf manchen Proben hinwies, lies auf einen möglichen Einfluss auf das Relaxationsverhalten und die Oberflächenrauhigkeit schließen. / Several thin InN and GaN/InN films and (In, Ga)N heterostructures were grown using molecular beam epitaxy to investigate their growth mode. InN and GaN/InN films were grown on ZnO substrates and (In, Ga)N heterostructures were grown on (In, Ga)N buffers and ZnO substrates. Fabricating the heterostructures on two different types of substrates was a means of strain engineering to possibly increase the indium content in the (In, Ga)N layers. An annealing procedure was established to treat ZnO substrate to gain smooth, stepped surfaces suitable for ML thin heterostructure devices. Reflection high energy electron diffraction was used to investigate in situ the growth mechanism and evolution of the a-lattice spacing. The critical layer thickness for growth mode transition of InN from smooth to rough is below 2 MLs and fairly coincides with the onset of main relaxation. The deposition of GaN on ML thin InN/ZnO shows that at best a few MLs can be deposited before relaxation and/or intermixing into (In, GaN) takes place. Investigations by X-ray diffraction and Raman spectroscopy indicate that the deposition of a nominal structure of 100x(1 ML InN/2 MLs GaN) seems to result in the growth of (In, Ga)N instead. The average chemical composition was similar for all samples with an indium content close to x: 0.36 and a degree of relaxation between 65%-73% for samples grown on ZnO and 95% for the sample grown on 300 nm In0.19Ga0.81N/GaN pseudo-substrate. The surface was probed with atomic force microscopy and showed that starting with smooth surfaces with root mean square roughness around 0.2 nm there was a considerable roughening during growth and surfaces with grain like morphology and a roughness around 2 to 3 nm was produced. Unintentional differences in V/III ratio during growth of (In, Ga)N heterostructures, indicated by the presence of droplets on some of the sample surfaces, were possible, impacting on the sample relaxation behavior and the surface roughness.

No description available.

No description available.

No description available.