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Lawler, Michael Joseph ; Winkler, Paul M. ; Kim, Jaeseok ; Ahlm, Lars ; Tröstl, Jasmin ; Praplan, Arnaud Patrick ; Schobesberger, Siegfried ; Kürten, Christoph Andreas ; Kirkby, Jasper ; Bianchi, Federico ; Duplissy, Jonathan ; Hansel, Armin ; Jokinen, Tuija ; Keskinen, Helmi ; Lehtipalo, Katrianne ; Leiminger, Markus ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Simon, Mario ; Sipilä, Mikko ; Williamson, Christina ; Wimmer, Daniela ; Riipinen, Ilona ; Virtanen, Annele ; Smith, James N.
New particle formation driven by acid–base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas-phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas-phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10–30 nm VMD particles. This behavior is not consistent with present nanoparticle physicochemical models, which predict a higher dimethylaminium fraction when NH3 and DMA are present at similar gas-phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base : acid ratios lower than 1 : 1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient. The reasons for the very acidic composition remain uncertain, but a plausible explanation is that the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO2 to sulfate. These results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid–base pairs in particles as small as 10 nm.
Plank, Harald ; Winkler, Robert ; Schwalb, Christian H. ; Hütner, Johanna ; Fowlkes, Jason D. ; Rack, Philip D. ; Utke, Ivo ; Huth, Michael
Scanning probe microscopy (SPM) has become an essential surface characterization technique in research and development. By concept, SPM performance crucially depends on the quality of the nano-probe element, in particular, the apex radius. Now, with the development of advanced SPM modes beyond morphology mapping, new challenges have emerged regarding the design, morphology, function, and reliability of nano-probes. To tackle these challenges, versatile fabrication methods for precise nano-fabrication are needed. Aside from well-established technologies for SPM nano-probe fabrication, focused electron beam-induced deposition (FEBID) has become increasingly relevant in recent years, with the demonstration of controlled 3D nanoscale deposition and tailored deposit chemistry. Moreover, FEBID is compatible with practically any given surface morphology. In this review article, we introduce the technology, with a focus on the most relevant demands (shapes, feature size, materials and functionalities, substrate demands, and scalability), discuss the opportunities and challenges, and rationalize how those can be useful for advanced SPM applications. As will be shown, FEBID is an ideal tool for fabrication/modification and rapid prototyping of SPM-tipswith the potential to scale up industrially relevant manufacturing.