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- ItemExtreme events in gross primary production: A characterization across continents(MĆ¼nchen : European Geopyhsical Union, 2014) Zscheischler, J.; Reichstein, M.; Harmeling, S.; Rammig, A.; Tomelleri, E.; Mahecha, M.D.Climate extremes can affect the functioning of terrestrial ecosystems, for instance via a reduction of the photosynthetic capacity or alterations of respiratory processes. Yet the dominant regional and seasonal effects of hydrometeorological extremes are still not well documented and in the focus of this paper. Specifically, we quantify and characterize the role of large spatiotemporal extreme events in gross primary production (GPP) as triggers of continental anomalies. We also investigate seasonal dynamics of extreme impacts on continental GPP anomalies. We find that the 50 largest positive extremes (i.e., statistically unusual increases in carbon uptake rates) and negative extremes (i.e., statistically unusual decreases in carbon uptake rates) on each continent can explain most of the continental variation in GPP, which is in line with previous results obtained at the global scale. We show that negative extremes are larger than positive ones and demonstrate that this asymmetry is particularly strong in South America and Europe. Our analysis indicates that the overall impacts and the spatial extents of GPP extremes are power-law distributed with exponents that vary little across continents. Moreover, we show that on all continents and for all data sets the spatial extents play a more important role for the overall impact of GPP extremes compared to the durations or maximal GPP. An analysis of possible causes across continents indicates that most negative extremes in GPP can be attributed clearly to water scarcity, whereas extreme temperatures play a secondary role. However, for Europe, South America and Oceania we also identify fire as an important driver. Our findings are consistent with remote sensing products. An independent validation against a literature survey on specific extreme events supports our results to a large extent.
- ItemUnderstanding aerosol microphysical properties from 10 years of data collected at Cabo Verde based on an unsupervised machine learning classification(Katlenburg-Lindau : EGU, 2022) Gong, Xianda; Wex, Heike; MĆ¼ller, Thomas; Henning, Silvia; VoigtlƤnder, Jens; Wiedensohler, Alfred; Stratmann, FrankThe Cape Verde Atmospheric Observatory (CVAO), which is influenced by both marine and desert dust air masses, has been used for long-term measurements of different properties of the atmospheric aerosol from 2008 to 2017. These properties include particle number size distributions (PNSD), light-absorbing carbon (LAC) and concentrations of cloud condensation nuclei (CCN) together with their hygroscopicity. Here we summarize the results obtained for these properties and use an unsupervised machine learning algorithm for the classification of aerosol types. Five types of aerosols, i.e., marine, freshly formed, mixture, moderate dust and heavy dust, were classified. Air masses during marine periods are from the Atlantic Ocean and during dust periods are from the Sahara Desert. Heavy dust was more frequently present during wintertime, whereas the clean marine periods were more frequently present during springtime. It was observed that during the dust periods CCN number concentrations at a supersaturation of 0.30g% were roughly 2.5 times higher than during marine periods, but the hygroscopicity (Īŗ) of particles in the size range from g1/4g30 to g1/4g175gnm during marine and dust periods were comparable. The long-term data presented here, together with the aerosol classification, can be used as a basis to improve our understanding of annual cycles of the atmospheric aerosol in the eastern tropical Atlantic Ocean and on aerosol-cloud interactions and it can be used as a basis for driving, evaluating and constraining atmospheric model simulations.
- ItemGrowth and Properties of Intentionally Carbon-Doped GaN Layers(Weinheim : Wiley-VCH, 2019) Richter, Eberhard; Beyer, Franziska C.; Zimmermann, Friederike; GƤrtner, GĆ¼nter; Irmscher, Klaus; Gamov, Ivan; Heitmann, Johannes; Weyers, Markus; TrƤnkle, GĆ¼ntherCarbon-doping of GaN layers with thickness in the mm-range is performed by hydride vapor phase epitaxy. Characterization by optical and electrical measurements reveals semi-insulating behavior with a maximum of specific resistivity of 2 Ć 1010 Ī© cm at room temperature found for a carbon concentration of 8.8 Ć 1018 cmā3. For higher carbon levels up to 3.5 Ć 1019 cmā3, a slight increase of the conductivity is observed and related to self-compensation and passivation of the acceptor. The acceptor can be identified as CN with an electrical activation energy of 0.94 eV and partial passivation by interstitial hydrogen. In addition, two differently oriented tri-carbon defects, CN-a-CGa-a-CN and CN-a-CGa-c-CN, are identified which probably compensate about two-thirds of the carbon which is incorporated in excess of 2 Ć 1018 cmā3. Ā© 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemSc3CH@C80: selective 13C enrichment of the central carbon atom(Cambridge : Royal Society of Chemistry, 2016) Junghans, Katrin; Rosenkranz, Marco; Popov, Alexey A.Sc3CH@C80 is synthesized and characterized by 1H, 13C, and 45Sc NMR. A large negative chemical shift of the proton, -11.73 ppm in the Ih and -8.79 ppm in the D5h C80 cage isomers, is found. 13C satellites in the 1H NMR spectrum enabled indirect determination of the 13C chemical shift for the central carbon at 173 Ā± 1 ppm. Intensity of the satellites allowed determination of the 13C content for the central carbon atom. This unique possibility is applied to analyze the cluster/cage 13C distribution in mechanistic studies employing either 13CH4 or 13C powder to enrich Sc3CH@C80 with 13C.
- ItemHydrophilic non-precious metal nitrogen-doped carbon electrocatalysts for enhanced efficiency in oxygen reduction reaction(Cambridge : Royal Society of Chemistry, 2015) Hao, Guang-Ping; Sahraie, Nastaran Ranjbar; Zhang, Qiang; Krause, Simon; Oschatz, Martin; Bachmatiuk, Alicja; Strasser, Peter; Kaskel, StefanExploring the role of surface hydrophilicity of non-precious metal N-doped carbon electrocatalysts in electrocatalysis is challenging. Herein we discover an ultra-hydrophilic non-precious carbon electrocatalyst, showing enhanced catalysis efficiency on both gravimetric and areal basis for oxygen reduction reaction due to a high dispersion of active centres.
- ItemManganese-catalyzed selective CāH activation and deuteration by means of a catalytic transient directing group strategy(London : Royal Society of Chemistry (RSC), 2021) Kopf, Sara; Neumann, Helfried; Beller, MatthiasA novel manganese-catalyzed C-H activation methodology for selective hydrogen isotope exchange of benzaldehydes is presented. Using D2O as a cheap and convenient source of deuterium, the reaction proceeds with excellent functional group tolerance. Highortho-selectivity is achieved in the presence of catalytic amounts of specific amines, whichin situform a transient directing group. Ā© The Royal Society of Chemistry 2021.
- ItemQuinone-decorated onion-like carbon/carbon fiber hybrid electrodes for high-rate supercapacitor applications(Hoboken, NJ : Wiley, 2015) Zeiger, Marco; Weingarth, Daniel; Presser, VolkerThe energy performance of carbon onions can be significantly enhanced by introducing pseudocapacitive materials, but this is commonly at the cost of power handling. In this study, a novel synergistic electrode preparation method was developed by using carbon-fiber substrates loaded with quinone-decorated carbon onions. The electrodes are free standing, binder free, extremely conductive, and the interfiber space filling overcomes the severely low apparent density commonly found for electrospun fibers. Electrochemical measurements were performed in organic and aqueous electrolytes. For both systems, a high electrochemical stability after 10ā000 cycles was measured, as well as a long-term voltage floating test for the organic electrolyte. The capacitance in 1āM H2SO4 was 288ā Fāg^ā1 for the highest loading of quinones, which is similar to literature values, but with a very high power handling, showing more than 100ā Fāg^ā1 at a scan rate of 2ā Vs^ā1.
- ItemTriangular Monometallic Cyanide Cluster Entrapped in Carbon Cage with Geometry-Dependent Molecular Magnetism(Washington, DC : ACS Publications, 2016) Liu, Fupin; Gao, Cong-Li; Deng, Qingming; Zhu, Xianjun; Kostanyan, Aram; Westerstrƶm, Rasmus; Wang, Song; Tan, Yuan-Zhi; Tao, Jun; Xie, Su-Yuan; Popov, Alexey A.; Greber, Thomas; Yang, ShangfengClusterfullerenes are capable of entrapping a variety of metal clusters within carbon cage, for which the entrapped metal cluster generally keeps its geometric structure (e.g., bond distance and angle) upon changing the isomeric structure of fullerene cage, and whether the properties of the entrapped metal cluster is geometry-dependent remains unclear. Herein we report an unusual triangular monometallic cluster entrapped in fullerene cage by isolating several novel terbium cyanide clusterfullerenes (TbNC@C82) with different cage isomeric structures. Upon varying the isomeric structure of C82 cage from C2(5) to Cs(6) and to C2v(9), the entrapped triangular TbNC cluster exhibits significant distortions as evidenced by the changes of TbāC(N) and CāN bond distances and variation of the TbāC(N)āN(C) angle by up to 20Ā°, revealing that the geometric structure of the entrapped triangular TbNC cluster is variable. All three TbNC@C82 molecules are found to be single-ion magnets, and the change of the geometric structure of TbNC cluster directly leads to the alternation of the magnetic relaxation time of the corresponding TbNC@C82 clusterfullerene.
- ItemProximal Soil Sensing - A Contribution for Species Habitat Distribution Modelling of Earthworms in Agricultural Soils?(San Francisco, California, US : PLOS, 2016) Schirrmann, Michael; Joschko, Monika; Gebbers, Robin; Kramer, Eckart; Zƶrner, Mirjam; Barkusky, Dietmar; Timmer, JensBackground: Earthworms are important for maintaining soil ecosystem functioning and serve as indicators of soil fertility. However, detection of earthworms is time-consuming, which hinders the assessment of earthworm abundances with high sampling density over entire fields. Recent developments of mobile terrestrial sensor platforms for proximal soil sensing (PSS) provided new tools for collecting dense spatial information of soils using various sensing principles. Yet, the potential of PSS for assessing earthworm habitats is largely unexplored. This study investigates whether PSS data contribute to the spatial prediction of earthworm abundances in species distribution models of agricultural soils. Methodology/Principal Findings: Proximal soil sensing data, e.g., soil electrical conductivity (EC), pH, and near infrared absorbance (NIR), were collected in real-time in a field with two management strategies (reduced tillage / conventional tillage) and sandy to loam soils. PSS was related to observations from a long-term (11 years) earthworm observation study conducted at 42 plots. Earthworms were sampled from 0.5 x 0.5 x 0.2 mĀ³ soil blocks and identified to species level. Sensor data were highly correlated with earthworm abundances observed in reduced tillage but less correlated with earthworm abundances observed in conventional tillage. This may indicate that management influences the sensor-earthworm relationship. Generalized additive models and state-space models showed that modelling based on data fusion from EC, pH, and NIR sensors produced better results than modelling without sensor data or data from just a single sensor. Regarding the individual earthworm species, particular sensor combinations were more appropriate than others due to the different habitat requirements of the earthworms. Earthworm species with soil-specific habitat preferences were spatially predicted with higher accuracy by PSS than more ubiquitous species. Conclusions/Significance: Our findings suggest that PSS contributes to the spatial modelling of earthworm abundances at field scale and that it will support species distribution modelling in the attempt to understand the soil-earthworm relationships in agroecosystems.
- ItemCurrent Status of CarbonāRelated Defect Luminescence in GaN(Weinheim : Wiley-VCH, 2021) Zimmermann, Friederike; Beyer, Jan; Rƶder, Christian; Beyer, Franziska C.; Richter, Eberhard; Irmscher, Klaus; Heitmann, JohannesHighly insulating layers are a prerequisite for gallium nitride (GaN)-based power electronic devices. For this purpose, carbon doping is one of the currently pursued approaches. However, its impact on the optical and electrical properties of GaN has been widely debated in the scientific community. For further improvement of device performance, a better understanding of the role of related defects is essential. To study optically active point defects, photoluminescence is one of the most frequently used experimental characterization techniques. Herein, the main recent advances in the attribution of carbon-related photoluminescence bands are reviewed, which were enabled by the interplay of a refinement of growth and characterization techniques and state-of-the-art first-principles calculations developed during the last decade. The predicted electronic structures of isolated carbon defects and selected carbon-impurity complexes are compared to experimental results. Taking into account both of these, a comprehensive overview on the present state of interpretation of carbon-related broad luminescence bands in bulk GaN is presented.