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- ItemInfluences of the 2010 Eyjafjallajökull volcanic plume on air quality in the northern Alpine region(München : European Geopyhsical Union, 2011) Schäfer, K.; Thomas, W.; Peters, A.; Ries, L.; Obleitner, F.; Schnelle-Kreis, J.; Birmili, W.; Diemer, J.; Fricke, W.; Junkermann, W.; Pitz, M.; Emeis, S.; Forkel, R.; Suppan, P.; Flentje, H.; Gilge, S.; Wichmann, H.E.; Meinhardt, F.; Zimmermann, R.; Weinhold, K.; Soentgen, J.; Münkel, C.; Freuer, C.; Cyrys, J.A series of major eruptions of the Eyjafjallajökull volcano in Iceland started on 14 April 2010 and continued until the end of May 2010. The volcanic emissions moved over nearly the whole of Europe and were observed first on 16 April 2010 in Southern Germany with different remote sensing systems from the ground and space. Enhanced PM10 and SO2 concentrations were detected on 17 April at mountain stations (Zugspitze/Schneefernerhaus and Schauinsland) as well as in Innsbruck by in situ measurement devices. On 19 April intensive vertical mixing and advection along with clear-sky conditions facilitated the entrainment of volcanic material down to the ground. The subsequent formation of a stably stratified lower atmosphere with limited mixing near the ground during the evening of 19 April led to an additional enhancement of near-surface particle concentrations. Consequently, on 19 April and 20 April exceedances of the daily threshold value for particulate matter (PM10) were reported at nearly all monitoring stations of the North Alpine foothills as well as at mountain and valley stations in the northern Alps. The chemical analyses of ambient PM10 at monitoring stations of the North Alpine foothills yielded elevated Titanium concentrations on 19/20 April which prove the presence of volcanic plume material. Following this result the PM10 threshold exceedances are also associated with the volcanic plume. The entrainment of the volcanic plume material mainly affected the concentrations of coarse particles (>1 μm) – interpreted as volcanic ash – and ultrafine particles (<100 nm), while the concentrations of accumulation mode aerosol (0.1–1 μm) were not changed significantly. With regard to the occurrence of ultrafine particles, it is concluded that their formation was triggered by high sulphuric acid concentrations which are necessarily generated by the photochemical processes in a plume rich in sulphur dioxide under high solar irradiance. It became evident that during the course of several days, the Eyjafjallajökull volcanic emissions influenced the near-surface atmosphere and thus the ambient air quality. Although the volcanic plume contributed to the overall exposure of the population of the northern Alpine region on two days, only minor effects on the exacerbation of respiratory and cardiovascular symptoms can be expected.
- ItemA thiazolo[5,4-: D] thiazole-bridged porphyrin organic framework as a promising nonlinear optical material(London : Royal Society of Chemistry (RSC), 2019) Samal, Mahalaxmi; Valligatla, Sreeramulu; Saad, Nabil A.; Rao, M. Veeramohan; Rao, D. Narayana; Sahu, Rojalin; Biswal, Bishnu P.Porphyrin-based porous organic frameworks are an important group of materials gaining interest due to their structural diversity and distinct opto-electronic properties. However, these materials are seldom explored for nonlinear optical (NLO) applications. In this work, we investigate a thiazolo[5,4-d]thiazole-bridged porous, porphyrin framework (Por-TzTz-POF) with promising NLO properties. The planar TzTz moiety coupled with integrated porphyrin units enables efficient π-conjugation and charge distribution in the Por-TzTz-POF resulting in a high nonlinear absorption coefficient (β = 1100 cm GW-1) with figure of merit (FoM) σ1/σ0 = 5571, in contrast to analogous molecules and material counterparts e.g. metal-organic frameworks (MOFs; β = ∼0.3-0.5 cm GW-1), molecular porphyrins (β = ∼100-400 cm GW-1), graphene (β = 900 cm GW-1), and covalent organic frameworks (Por-COF-HH; β = 1040 cm GW-1 and FoM = 3534). This journal is © The Royal Society of Chemistry.
- ItemProduction of highly concentrated and hyperpolarized metabolites within seconds in high and low magnetic fields(Cambridge : RSC Publ., 2019) Korchak, Sergey; Emondts, Meike; Mamone, Salvatore; Blümich, Bernhard; Glöggler, StefanHyperpolarized metabolites are very attractive contrast agents for in vivo magnetic resonance imaging studies enabling early diagnosis of cancer, for example. Real-time production of concentrated solutions of metabolites is a desired goal that will enable new applications such as the continuous investigation of metabolic changes. To this end, we are introducing two NMR experiments that allow us to deliver high levels of polarization at high concentrations (50 mM) of an acetate precursor (55% 13C polarization) and acetate (17% 13C polarization) utilizing 83% para-state enriched hydrogen within seconds at high magnetic field (7 T). Furthermore, we have translated these experiments to a portable low-field spectrometer with a permanent magnet operating at 1 T. The presented developments pave the way for a rapid and affordable production of hyperpolarized metabolites that can be implemented in e.g. metabolomics labs and for medical diagnosis.
- ItemResonating holes vs molecular spin-orbit coupled states in group-5 lacunar spinels([London] : Nature Publishing Group UK, 2023) Petersen, Thorben; Bhattacharyya, Pritam; Rößler, Ulrich K.; Hozoi, LiviuThe valence electronic structure of magnetic centers is one of the factors that determines the characteristics of a magnet. This may refer to orbital degeneracy, as for jeff = 1/2 Kitaev magnets, or near-degeneracy, e.g., involving the third and fourth shells in cuprate superconductors. Here we explore the inner structure of magnetic moments in group-5 lacunar spinels, fascinating materials featuring multisite magnetic units in the form of tetrahedral tetramers. Our quantum chemical analysis reveals a very colorful landscape, much richer than the single-electron, single-configuration description applied so far to all group-5 GaM4X8 chalcogenides, and clarifies the basic multiorbital correlations on M4 tetrahedral clusters: while for V strong correlations yield a wave-function that can be well described in terms of four V4+V3+V3+V3+ resonant valence structures, for Nb and Ta a picture of dressed molecular-orbital jeff = 3/2 entities is more appropriate. These internal degrees of freedom likely shape vibronic couplings, phase transitions, and the magneto-electric properties in each of these systems.
- ItemStructure formation of ultrathin PEO films at solid interfaces-complex pattern formation by dewetting and crystallization(Basel : MDPI AG, 2013) Braun, H.-G.; Meyer, E.The direct contact of ultrathin polymer films with a solid substrate may result in thin film rupture caused by dewetting. With crystallisable polymers such as polyethyleneoxide (PEO), molecular self-assembly into partial ordered lamella structures is studied as an additional source of pattern formation. Morphological features in ultrathin PEO films (thickness < 10 nm) result from an interplay between dewetting patterns and diffusion limited growth pattern of ordered lamella growing within the dewetting areas. Besides structure formation of hydrophilic PEO molecules, n-alkylterminated (hydrophobic) PEO oligomers are investigated with respect to self-organization in ultrathin films. Morphological features characteristic for pure PEO are not changed by the presence of the n-alkylgroups.
- ItemTwo types of magnetic shape-memory effects from twinned microstructure and magneto-structural coupling in Fe1 +yTe(Washington : National Academy of Sciences, 2019) Rößler, S.; Koz, C.; Wang, Z.; Skourski, Y.; Doerr, M.; Kasinathan, D.; Rosner, H.; Schmidt, M.; Schwarz, U.; Rößler, U.K.; Wirth, S.A detailed experimental investigation of Fe1+yTe (y = 0.11, 0.12) using pulsed magnetic fields up to 60 T confirms remarkable magnetic shape-memory (MSM) effects. These effects result from magnetoelastic transformation processes in the low-temperature antiferromagnetic state of these materials. The observation of modulated and finely twinned microstructure at the nanoscale through scanning tunneling microscopy establishes a behavior similar to that of thermoelastic martensite. We identified the observed, elegant hierarchical twinning pattern of monoclinic crystallographic domains as an ideal realization of crossing twin bands. The antiferromagnetism of the monoclinic ground state allows for a magnetic-field–induced reorientation of these twin variants by the motion of one type of twin boundaries. At sufficiently high magnetic fields, we observed a second isothermal transformation process with large hysteresis for different directions of applied field. This gives rise to a second MSM effect caused by a phase transition back to the field-polarized tetragonal lattice state.
- ItemNew insights in sources of the sub-micrometre aerosol at Mt. Zeppelin observatory (Spitsbergen) in the year 2015(Stockholm : Stockholm University Press, 2019) Karl, Matthias; Leck, Caroline; Rad, Farshid Mashayekhy; Bäcklund, Are; Lopez-Aparicio, Susana; Heintzenberg, JostIn order to evaluate the potential impact of the Arctic anthropogenic emission sources it is essential to understand better the natural aerosol sources of the inner Arctic and the atmospheric processing of the aerosols during their transport in the Arctic atmosphere. A 1-year time series of chemically specific measurements of the sub-micrometre aerosol during 2015 has been taken at the Mt. Zeppelin observatory in the European Arctic. A source apportionment study combined measured molecular tracers as source markers, positive matrix factorization, analysis of the potential source distribution and auxiliary information from satellite data and ground-based observations. The annual average sub-micrometre mass was apportioned to regional background secondary sulphate (56%), sea spray (17%), biomass burning (15%), secondary nitrate (5.8%), secondary marine biogenic (4.5%), mixed combustion (1.6%), and two types of marine gel sources (together 0.7%). Secondary nitrate aerosol mainly contributed towards the end of summer and during autumn. During spring and summer, the secondary marine biogenic factor reached a contribution of up to 50% in some samples. The most likely origin of the mixed combustion source is due to oil and gas extraction activities in Eastern Siberia. The two marine polymer gel sources predominantly occurred in autumn and winter. The small contribution of the marine gel sources at Mt. Zeppelin observatory in summer as opposed to regions closer to the North Pole is attributed to differences in ocean biology, vertical distribution of phytoplankton, and the earlier start of the summer season.