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- ItemThe use of matrix-specific calibrations for oxygen in analytical glow discharge spectrometry(Dordrecht : Springer, 2014) Gonzalez-Gago, C.; Smid, P.; Hofmann, T.; Venzago, C.; Hoffmann, V.; Gruner, W.The performance of glow discharge optical emission spectroscopy and mass spectrometry for oxygen determination is investigated using a set of new conductive samples containing oxygen in the percent range in three different matrices (Al, Mg, and Cu) prepared by a sintering process. The sputtering rate corrected calibrations obtained at standard conditions for the 4 mm anode (700 V, 20 mA) in GD-OES are matrix independent for Mg and Al but not for Cu. The importance of a "blue shifted" line of oxygen at 130.22 nm (first reported by Köster) for quantitative analyses by GD-OES is confirmed. Matrix-specific calibrations for oxygen in GD-MS are presented. Two source concepts - fast flow (ELEMENT GD) and low gas flow (VG9000) - are evaluated obtaining higher sensitivity with the static flow source. Additional experiments using Ar-He mixtures or μs pulsed GD are carried out in ELEMENT GD aiming to improve the oxygen sensitivity.
- ItemOxygen-deficient oxide growth by subliming the oxide source material: The cause of silicide formation in rare earth oxides on silicon(Washington, DC : ACS, 2013) Bierwagen, O.; Proessdorf, A.; Niehle, M.; Grosse, F.; Trampert, A.; Klingsporn, M.The fundamental issue of oxygen stoichiometry in oxide thin film growth by subliming the source oxide is investigated by varying the additionally supplied oxygen during molecular beam epitaxy of RE2O3 (RE = Gd, La, Lu) thin films on Si(111). Supplying additional oxygen throughout the entire growth was found to prevent the formation of rare earth silicides observed in films grown without an oxygen source. Postgrowth vacuum annealing of oxygen stoichiometric films did not lead to silicide formation thereby confirming that the silicides do not form as a result of an interface instability at growth temperature in vacuum but rather due to an oxygen deficiency in the source vapor. The average oxygen deficiency of the rare-earth containing species in the source vapor was quantified by the 18O tracer technique and correlated with that of the source material, which gradually decomposed during sublimation. Therefore, any oxide growth by sublimation of the oxide source material requires additional oxygen to realize oxygen stoichiometric films.
- ItemHighly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol(Washington, DC : ACS Publ., 2019) Bianchi, Federico; Kurtén, Theo; Riva, Matthieu; Mohr, Claudia; Rissanen, Matti P.; Roldin, Pontus; Berndt, Torsten; Crounse, John D.; Wennberg, Paul O.; Mentel, Thomas F.; Wildt, Jürgen; Junninen, Heikki; Jokinen, Tuija; Kulmala, Markku; Worsnop, Douglas R.; Thornton, Joel A.; Donahue, Neil; Kjaergaard, Henrik G.; Ehn, MikaelHighly oxygenated organic molecules (HOM) are formed in the atmosphere via autoxidation involving peroxy radicals arising from volatile organic compounds (VOC). HOM condense on pre-existing particles and can be involved in new particle formation. HOM thus contribute to the formation of secondary organic aerosol (SOA), a significant and ubiquitous component of atmospheric aerosol known to affect the Earth's radiation balance. HOM were discovered only very recently, but the interest in these compounds has grown rapidly. In this Review, we define HOM and describe the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties. A main aim is to provide a common frame for the currently quite fragmented literature on HOM studies. Finally, we highlight the existing gaps in our understanding and suggest directions for future HOM research. © 2019 American Chemical Society.
- ItemRemarkable performance recovery in highly defective perovskite solar cells by photo-oxidation(London [u.a.] : RSC, 2023) Goetz, Katelyn P.; Thome, Fabian T. F.; An, Qingzhi; Hofstetter, Yvonne J.; Schramm, Tim; Yangui, Aymen; Kiligaridis, Alexander; Loeffler, Markus; Taylor, Alexander D.; Scheblykin, Ivan G.; Vaynzof, YanaExposure to environmental factors is generally expected to cause degradation in perovskite films and solar cells. Herein, we show that films with certain defect profiles can display the opposite effect, healing upon exposure to oxygen under illumination. We tune the iodine content of methylammonium lead triiodide perovskite from understoichiometric to overstoichiometric and expose them to oxygen and light prior to the addition of the top layers of the device, thereby examining the defect dependence of their photooxidative response in the absence of storage-related chemical processes. The contrast between the photovoltaic properties of the cells with different defects is stark. Understoichiometric samples indeed degrade, demonstrating performance at 33% of their untreated counterparts, while stoichiometric samples maintain their performance levels. Surprisingly, overstoichiometric samples, which show low current density and strong reverse hysteresis when untreated, heal to maximum performance levels (the same as untreated, stoichiometric samples) upon the photooxidative treatment. A similar, albeit smaller-scale, effect is observed for triple cation and methylammonium-free compositions, demonstrating the general application of this treatment to state-of-the-art compositions. We examine the reasons behind this response by a suite of characterization techniques, finding that the performance changes coincide with microstructural decay at the crystal surface, reorientation of the bulk crystal structure for the understoichiometric cells, and a decrease in the iodine-to-lead ratio of all films. These results indicate that defect engineering is a powerful tool to manipulate the stability of perovskite solar cells.
- ItemOn the Impact of Strained PECVD Oxide Layers on Oxide Precipitation in Silicon(Pennington, NJ : ECS, 2019) Kissinger, G.; Kot, D.; Lisker, M.; Sattler, A.PECVD oxide layers with different layer stress ranging from about −305.2 MPa to 39.9 MPa were deposited on silicon wafers with similar concentration of interstitial oxygen. After a thermal treatment consisting of rapid thermal annealing (RTA) and furnace annealing 780°C 3 h + 1000°C 16 h in nitrogen the profiles of the oxide precipitate density were investigated. Supersaturations of self-interstitials as function of layer stress were determined by adjusting modelling results to measured depth profiles of bulk microdefects. The self-interstitial supersaturation generated by RTA at 1250°C and 1175°C at the silicon/oxide interface is increasing linearly with increasing layer stress. Values for self-interstitial supersaturation determined on deposited oxide layers after RTA at 1250°C and 1175°C are very similar to values published for RTO by Sudo et al. An RTA at 1175°C with a PECVD oxide on top of the wafer is a method to effectively suppress oxygen precipitation in silicon wafers. Nucleation anneals carried out at 650°C for 4 h and 8 h did not show any effect of PECVD oxide layers on oxide precipitate nucleation. © The Author(s) 2019.
- ItemBiofunctionalized zinc peroxide (ZnO2) nanoparticles as active oxygen sources and antibacterial agents(London : RSC Publishing, 2017) Bergs, Christian; Brück, Lisa; Rosencrantz, Ruben R.; Conrads, Georg; Elling, Lothar; Pich, AndrijOxygen is one of the most important substances for physiological reactions and metabolisms in biological systems. Through the tailored design of oxygen-releasing materials it might be possible to control different biological processes. In this work we synthesized for the first time zinc peroxide nanoparticles with controlled sizes and biofunctionalized surfaces using a one-step reaction procedure. The zinc peroxide nanoparticles were obtained with tunable sizes (between 4.0 ± 1.2 nm and 9.4 ± 5.2 nm) and were decorated with glucose 1-phosphate (Glc-1P). The specific interaction of the phosphate function of Glc-1P with the nanoparticle surface was monitored by solid state 31P-NMR and zeta-potential measurements. Furthermore, using fluorescence measurements we demonstrated that anchored glucose molecules on the nanoparticle surface are accessible for specific interactions with lectins. It could be shown that these interactions strongly depend on the amount of Glc-1P attached to the nanoparticle surface. Additionally it was demonstrated that the oxygen release from biofunctionalized zinc peroxide nanoparticles could be tuned according to the chemical composition of the nanoparticles and the pH of the aqueous solution. The antibacterial efficiency of the synthesized nanoparticles against Enterococcus faecalis, Aggregatibacter actinomycetemcomitans, Porphyromonas gingivalis and Prevotella intermedia was evaluated by determination of minimal bactericidal concentration (MIC).
- ItemMicrobial respiration and natural attenuation of benzene contaminated soils investigated by cavity enhanced Raman multi-gas spectroscopy(Cambridge : Soc., 2015) Jochum, Tobias; Michalzik, Beate; Bachmann, Anne; Popp, Jürgen; Frosch, TorstenSoil and groundwater contamination with benzene can cause serious environmental damage. However, many soil microorganisms are capable to adapt and are known to strongly control the fate of organic contamination. Innovative cavity enhanced Raman multi-gas spectroscopy (CERS) was applied to investigate the short-term response of the soil micro-flora to sudden surface contamination with benzene regarding the temporal variations of gas products and their exchange rates with the adjacent atmosphere. 13C-labeled benzene was spiked on a silty-loamy soil column in order to track and separate the changes in heterotrophic soil respiration – involving 12CO2 and O2 – from the natural attenuation process of benzene degradation to ultimately form 13CO2. The respiratory quotient (RQ) decreased from a value 0.98 to 0.46 directly after the spiking and increased again within 33 hours to a value of 0.72. This coincided with the maximum 13CO2 concentration rate (0.63 μmol m−2 s−1), indicating the highest benzene degradation at 33 hours after the spiking event. The diffusion of benzene in the headspace and the biodegradation into 13CO2 were simultaneously monitored and 12 days after the benzene spiking no measurable degradation was detected anymore. The RQ finally returned to a value of 0.96 demonstrating the reestablished aerobic respiration.