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- ItemVideo-rate multi-color structured illumination microscopy with simultaneous real-time reconstruction(Berlin : Nature Publishing, 2019) Markwirth, A; Lachetta, Mario; Mönkemöller, V.; Heintzmann, Rainer; Hübner, Wolfgang; Huser, Thomas; Müller, MarcelSuper-resolved structured illumination microscopy (SR-SIM) is among the fastest fluorescence microscopy techniques capable of surpassing the optical diffraction limit. Current custom-build instruments are able to deliver two-fold resolution enhancement with high acquisition speed. SR-SIM is usually a two-step process, with raw-data acquisition and subsequent, time-consuming post-processing for image reconstruction. In contrast, wide-field and (multi-spot) confocal techniques produce high-resolution images instantly. Such immediacy is also possible with SR-SIM, by tight integration of a video-rate capable SIM with fast reconstruction software. Here we present instant SR-SIM by VIGOR (Video-rate Immediate GPU-accelerated Open-Source Reconstruction). We demonstrate multi-color SR-SIM at video frame-rates, with less than 250 ms delay between measurement and reconstructed image display. This is achieved by modifying and extending high-speed SR-SIM image acquisition with a new, GPU-enhanced, network-enabled image-reconstruction software. We demonstrate high-speed surveying of biological samples in multiple colors and live imaging of moving mitochondria as an example of intracellular dynamics.
- ItemEnvironmental co-benefits and adverse side-effects of alternative power sector decarbonization strategies([London] : Nature Publishing Group UK, 2019) Luderer, Gunnar; Pehl, Michaja; Arvesen, Anders; Gibon, Thomas; Bodirsky, Benjamin L.; de Boer, Harmen Sytze; Fricko, Oliver; Hejazi, Mohamad; Humpenöder, Florian; Iyer, Gokul; Mima, Silvana; Mouratiadou, Ioanna; Pietzcker, Robert C.; Popp, Alexander; van den Berg, Maarten; van Vuuren, Detlef; Hertwich, Edgar G.A rapid and deep decarbonization of power supply worldwide is required to limit global warming to well below 2 °C. Beyond greenhouse gas emissions, the power sector is also responsible for numerous other environmental impacts. Here we combine scenarios from integrated assessment models with a forward-looking life-cycle assessment to explore how alternative technology choices in power sector decarbonization pathways compare in terms of non-climate environmental impacts at the system level. While all decarbonization pathways yield major environmental co-benefits, we find that the scale of co-benefits as well as profiles of adverse side-effects depend strongly on technology choice. Mitigation scenarios focusing on wind and solar power are more effective in reducing human health impacts compared to those with low renewable energy, while inducing a more pronounced shift away from fossil and toward mineral resource depletion. Conversely, non-climate ecosystem damages are highly uncertain but tend to increase, chiefly due to land requirements for bioenergy.
- ItemCellular responses to beating hydrogels to investigate mechanotransduction([London] : Nature Publishing Group UK, 2019) Chandorkar, Yashoda; Castro Nava, Arturo; Schweizerhof, Sjören; Van Dongen, Marcel; Haraszti, Tamás; Köhler, Jens; Zhang, Hang; Windoffer, Reinhard; Mourran, Ahmed; Möller, Martin; De Laporte, LauraCells feel the forces exerted on them by the surrounding extracellular matrix (ECM) environment and respond to them. While many cell fate processes are dictated by these forces, which are highly synchronized in space and time, abnormal force transduction is implicated in the progression of many diseases (muscular dystrophy, cancer). However, material platforms that enable transient, cyclic forces in vitro to recreate an in vivo-like scenario remain a challenge. Here, we report a hydrogel system that rapidly beats (actuates) with spatio-temporal control using a near infra-red light trigger. Small, user-defined mechanical forces (~nN) are exerted on cells growing on the hydrogel surface at frequencies up to 10 Hz, revealing insights into the effect of actuation on cell migration and the kinetics of reversible nuclear translocation of the mechanosensor protein myocardin related transcription factor A, depending on the actuation amplitude, duration and frequency.
- ItemHomogeneous cobalt-catalyzed reductive amination for synthesis of functionalized primary amines([London] : Nature Publishing Group UK, 2019) Murugesan, Kathiravan; Wei, Zhihong; Chandrashekhar, Vishwas G.; Neumann, Helfried; Spannenberg, Anke; Jiao, Haijun; Beller, Matthias; Jagadeesh, Rajenahally V.The development of earth abundant 3d metal-based catalysts continues to be an important goal of chemical research. In particular, the design of base metal complexes for reductive amination to produce primary amines remains as challenging. Here, we report the combination of cobalt and linear-triphos (bis(2-diphenylphosphinoethyl)phenylphosphine) as the molecularly-defined non-noble metal catalyst for the synthesis of linear and branched benzylic, heterocyclic and aliphatic primary amines from carbonyl compounds, gaseous ammonia and hydrogen in good to excellent yields. Noteworthy, this cobalt catalyst exhibits high selectivity and as a result the -NH2 moiety is introduced in functionalized and structurally diverse molecules. An inner-sphere mechanism on the basis of the mono-cationic [triphos-CoH]+ complex as active catalyst is proposed and supported with density functional theory computation on the doublet state potential free energy surface and H2 metathesis is found as the rate-determining step.
- ItemA meta-analysis of catalytic literature data reveals property-performance correlations for the OCM reaction([London] : Nature Publishing Group UK, 2019) Schmack, Roman; Friedrich, Alexandra; Kondratenko, Evgenii V.; Polte, Jörg; Werwatz, Axel; Kraehnert, RalphDecades of catalysis research have created vast amounts of experimental data. Within these data, new insights into property-performance correlations are hidden. However, the incomplete nature and undefined structure of the data has so far prevented comprehensive knowledge extraction. We propose a meta-analysis method that identifies correlations between a catalyst’s physico-chemical properties and its performance in a particular reaction. The method unites literature data with textbook knowledge and statistical tools. Starting from a researcher’s chemical intuition, a hypothesis is formulated and tested against the data for statistical significance. Iterative hypothesis refinement yields simple, robust and interpretable chemical models. The derived insights can guide new fundamental research and the discovery of improved catalysts. We demonstrate and validate the method for the oxidative coupling of methane (OCM). The final model indicates that only well-performing catalysts provide under reaction conditions two independent functionalities, i.e. a thermodynamically stable carbonate and a thermally stable oxide support.
- ItemAdaptive responses of animals to climate change are most likely insufficient([London] : Nature Publishing Group UK, 2019) Radchuk, Viktoriia; Reed, Thomas; Teplitsky, Céline; van de Pol, Martijn; Charmantier, Anne; Hassall, Christopher; AdamÃk, Peter; Adriaensen, Frank; Ahola, Markus P.; Arcese, Peter; Avilés, Jesús Miguel; Balbontin, Javier; Berg, Karl S.; Borras, Antoni; Burthe, Sarah; Clobert, Jean; Dehnhard, Nina; de Lope, Florentino; Dhondt, André A.; Dingemanse, Niels J.; Doi, Hideyuki; Eeva, Tapio; Fickel, Joerns; Filella, Iolanda; Fossøy, Frode; Goodenough, Anne E.; Hall, Stephen J. G.; Hansson, Bengt; Harris, Michael; Hasselquist, Dennis; Hickler, Thomas; Joshi, Jasmin; Kharouba, Heather; MartÃnez, Juan Gabriel; Mihoub, Jean-Baptiste; Mills, James A.; Molina-Morales, Mercedes; Moksnes, Arne; Ozgul, Arpat; Parejo, Deseada; Pilard, Philippe; Poisbleau, Maud; Rousset, Francois; Rödel, Mark-Oliver; Scott, David; Senar, Juan Carlos; Stefanescu, Constanti; Stokke, BÃ¥rd G.; Kusano, Tamotsu; Tarka, Maja; Tarwater, Corey E.; Thonicke, Kirsten; Thorley, Jack; Wilting, Andreas; Tryjanowski, Piotr; Merilä, Juha; Sheldon, Ben C.; Pape Møller, Anders; Matthysen, Erik; Janzen, Fredric; Dobson, F. Stephen; Visser, Marcel E.; Beissinger, Steven R.; Courtiol, Alexandre; Kramer-Schadt, StephanieBiological responses to climate change have been widely documented across taxa and regions, but it remains unclear whether species are maintaining a good match between phenotype and environment, i.e. whether observed trait changes are adaptive. Here we reviewed 10,090 abstracts and extracted data from 71 studies reported in 58 relevant publications, to assess quantitatively whether phenotypic trait changes associated with climate change are adaptive in animals. A meta-analysis focussing on birds, the taxon best represented in our dataset, suggests that global warming has not systematically affected morphological traits, but has advanced phenological traits. We demonstrate that these advances are adaptive for some species, but imperfect as evidenced by the observed consistent selection for earlier timing. Application of a theoretical model indicates that the evolutionary load imposed by incomplete adaptive responses to ongoing climate change may already be threatening the persistence of species. © 2019, The Author(s).
- ItemFew-cycle laser driven reaction nanoscopy on aerosolized silica nanoparticles([London] : Nature Publishing Group UK, 2019) Rupp, Philipp; Burger, Christian; Kling, Nora G; Kübel, Matthias; Mitra, Sambit; Rosenberger, Philipp; Weatherby, Thomas; Saito, Nariyuki; Itatani, Jiro; Alnaser, Ali S.; Raschke, Markus B.; Rühl, Eckart; Schlander, Annika; Gallei, Markus; Seiffert, Lennart; Fennel, Thomas; Bergues, Boris; Kling, Matthias F.Nanoparticles offer unique properties as photocatalysts with large surface areas. Under irradiation with light, the associated near-fields can induce, enhance, and control molecular adsorbate reactions on the nanoscale. So far, however, there is no simple method available to spatially resolve the near-field induced reaction yield on the surface of nanoparticles. Here we close this gap by introducing reaction nanoscopy based on three-dimensional momentum-resolved photoionization. The technique is demonstrated for the spatially selective proton generation in few-cycle laser-induced dissociative ionization of ethanol and water on SiO2 nanoparticles, resolving a pronounced variation across the particle surface. The results are modeled and reproduced qualitatively by electrostatic and quasi-classical mean-field Mie Monte-Carlo (M3C) calculations. Reaction nanoscopy is suited for a wide range of isolated nanosystems and can provide spatially resolved ultrafast reaction dynamics on nanoparticles, clusters, and droplets.
- ItemInferring causation from time series in Earth system sciences([London] : Nature Publishing Group UK, 2019) Runge, Jakob; Bathiany, Sebastian; Bollt, Erik; Camps-Valls, Gustau; Coumou, Dim; Deyle, Ethan; Glymour, Clark; Kretschmer, Marlene; Mahecha, Miguel D.; Muñoz-MarÃ, Jordi; van Nes, Egbert H.; Peters, Jonas; Quax, Rick; Reichstein, Markus; Scheffer, Marten; Schölkopf, Bernhard; Spirtes, Peter; Sugihara, George; Sun, Jie; Zhang, Kun; Zscheischler, JakobThe heart of the scientific enterprise is a rational effort to understand the causes behind the phenomena we observe. In large-scale complex dynamical systems such as the Earth system, real experiments are rarely feasible. However, a rapidly increasing amount of observational and simulated data opens up the use of novel data-driven causal methods beyond the commonly adopted correlation techniques. Here, we give an overview of causal inference frameworks and identify promising generic application cases common in Earth system sciences and beyond. We discuss challenges and initiate the benchmark platform causeme.net to close the gap between method users and developers. © 2019, The Author(s).
- ItemKey determinants of global land-use projections([London] : Nature Publishing Group UK, 2019) Stehfest, Elke; van Zeist, Willem-Jan; Valin, Hugo; Havlik, Petr; Popp, Alexander; Kyle, Page; Tabeau, Andrzej; Mason-D’Croz, Daniel; Hasegawa, Tomoko; Bodirsky, Benjamin L.; Calvin, Katherine; Doelman, Jonathan C.; Fujimori, Shinichiro; Humpenöder, Florian; Lotze-Campen, Hermann; van Meijl, Hans; Wiebe, KeithLand use is at the core of various sustainable development goals. Long-term climate foresight studies have structured their recent analyses around five socio-economic pathways (SSPs), with consistent storylines of future macroeconomic and societal developments; however, model quantification of these scenarios shows substantial heterogeneity in land-use projections. Here we build on a recently developed sensitivity approach to identify how future land use depends on six distinct socio-economic drivers (population, wealth, consumption preferences, agricultural productivity, land-use regulation, and trade) and their interactions. Spread across models arises mostly from diverging sensitivities to long-term drivers and from various representations of land-use regulation and trade, calling for reconciliation efforts and more empirical research. Most influential determinants for future cropland and pasture extent are population and agricultural efficiency. Furthermore, land-use regulation and consumption changes can play a key role in reducing both land use and food-security risks, and need to be central elements in sustainable development strategies.
- ItemEffects of changing population or density on urban carbon dioxide emissions([London] : Nature Publishing Group UK, 2019) Ribeiro, Haroldo V.; Rybski, Diego; Kropp, Jürgen P.The question of whether urbanization contributes to increasing carbon dioxide emissions has been mainly investigated via scaling relationships with population or population density. However, these approaches overlook the correlations between population and area, and ignore possible interactions between these quantities. Here, we propose a generalized framework that simultaneously considers the effects of population and area along with possible interactions between these urban metrics. Our results significantly improve the description of emissions and reveal the coupled role between population and density on emissions. These models show that variations in emissions associated with proportionate changes in population or density may not only depend on the magnitude of these changes but also on the initial values of these quantities. For US areas, the larger the city, the higher is the impact of changing its population or density on its emissions; but population changes always have a greater effect on emissions than population density.