Chemical Mechanism Development: Laboratory Studies and Model Applications     

Harald Geiger  Ian Barnes  Karl H. Becker  Birger Bohn  Theo Brauers  Birgit Donner  Hans-Peter Dorn  Manfred Elend  Carlos M. Freitas Dinis  Dirk Grossmann  Heinz Hass  Holger Hein  Axel Hoffmann  Lars Hoppe  Frank Hülsemann  Dieter Kley  Björn Klotz  Hans G. Libuda  Tobias Maurer  Djuro Mihelcic  Geert K. Moortgat  Romeo Olariu  Peter Neeb  Dirk Poppe  Lars Ruppert  Claudia G. Sauer  Oleg Shestakov  Holger Somnitz  William R. Stockwell  Lars P. Thüner  Andreas Wahner  Peter Wiesen  Friedhelm Zabel  Reinhard Zellner  Cornelius Zetzsch 《Journal of Atmospheric Chemistry》2002,42(1):323-357

Within the German Tropospheric Research Programme (TFS) numerous kinetic and mechanistic studies on the tropospheric reaction/degradation of the following reactants were carried out: oxygenated VOC, aromatic VOC, biogenic VOC, short-lived intermediates, such as alkoxy and alkylperoxy radicals.At the conception of the projects these selected groups were classes of VOC or intermediates for which the atmospheric oxidation mechanisms were either poorly characterised or totally unknown. The motivation for these studies was the attainment of significant improvements in our understanding of the atmospheric chemical oxidation processes of these compounds, particularly with respect to their involvement in photooxidant formation in the troposphere. In the present paper the types of experimental investigations performed and the results obtained within the various projects are briefly summarised. The major achievements are highlighted and discussed in terms of their contribution to improving our understanding of the chemical processes controlling photosmog formation in the troposphere.  相似文献   

Modulation and symmetry changes in stellar dynamos     

E. Knobloch  S. M. Tobias  & N. O. Weiss 《Monthly notices of the Royal Astronomical Society》1998,297(4):1123-1138

Stellar dynamos are governed by non-linear partial differential equations (PDEs) which admit solutions with dipole, quadrupole or mixed symmetry (i.e. with different parities). These PDEs possess periodic solutions that describe magnetic cycles, and numerical studies reveal two different types of modulation. For modulations of Type 1 there are parity changes without significant changes of amplitude, while for Type 2 there are amplitude changes without significant changes in parity. In stars like the Sun, cyclic magnetic activity is interrupted by grand minima that correspond to Type 2 modulation. Although the Sun's magnetic field has maintained dipole symmetry for almost 300 yr, there was a significant parity change at the end of the Maunder Minimum. We infer that the solar field may have flipped from dipole to quadrupole polarity (and back) after deep minima in the past and may do so again in the future. Other stars, with different masses or rotation rates, may exhibit cyclic activity with dipole, quadrupole or mixed parity. The origins of such behaviour can be understood by relating the PDE results to solutions of appropriate low-order systems of ordinary differential equations (ODEs). Type 1 modulation is reproduced in a fourth-order system while Type 2 modulation occurs in a third-order system. Here we construct a new sixth-order system that describes both types of modulation and clarifies the interactions between symmetry-breaking and modulation of activity. Solutions of these non-linear ODEs reproduce the qualitative behaviour found for the PDEs, including flipping of polarity after a prolonged grand minimum. Thus we can be confident that these patterns of behaviour are robust, and will apply to stars that are similar to the Sun.  相似文献   

Using archaeological data and sediment parameters to review the formation of the Gravettian layers at Krems-Wachtberg     

Marc Händel  Roswitha Thomas  Tobias Sprafke  Philipp Schulte  Michael Brandl  Ulrich Simon  Thomas Einwögerer 《第四纪科学杂志》2021,36(8):1397-1413

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Angular momentum transport and disc morphology in smoothed particle hydrodynamics simulations of galaxy formation     

Tobias Kaufmann  Lucio Mayer  James Wadsley  Joachim Stadel  Ben Moore 《Monthly notices of the Royal Astronomical Society》2007,375(1):53-67

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Mineralization of vestimentiferan tubes at methane seeps on the Congo deep-sea fan     

Antonie Haas  Crispin T.S. Little  Heiko Sahling  Gerhard Bohrmann  Tobias Himmler  Jörn Peckmann 《Deep Sea Research Part I: Oceanographic Research Papers》2009,56(2):283-293

Vestimentiferan tube worms are prominent members of modern methane seep communities and are totally reliant as adults on symbiotic sulphide-oxidizing bacteria for their nutrition. The sulphide is produced in the sediment by a biochemical reaction called the anaerobic oxidation of methane (AOM). A well-studied species from the Gulf of Mexico shows that seep vestimentiferans ‘mine’ sulphide from the sediment using root-like, thin walled, permeable posterior tube extensions, which can also be used to pump sulphate and possibly hydrogen ions from the soft tissue back into the sediment to increase the local rate of AOM. The ‘root-balls’ of exhumed seep vestimentiferans are intimately associated with carbonate nodules, which are a result of AOM. We have studied vestimentiferan specimens and associated carbonates from seeps at the Kouilou pockmark field on the Congo deep-sea fan and find that some of the posterior ‘root’ tubes of living specimens are enclosed with carbonate indurated sediment and other, empty examples are partially or completely replaced by the carbonate mineral aragonite. This replacement occurs from the outside of the tube wall inwards and leaves fine-scale relict textures of the original organic tube wall. The process of mineralization is unknown, but is likely a result of post-mortem microbial decay of the tube wall proteins by microorganisms or the precipitation from locally high flux of AOM derived carbonate ions. The aragonite-replaced tubes from the Kouilou pockmarks show similar features to carbonate tubes in ancient seep deposits and make it more likely that many of these fossil tubes are those of vestimentiferans. These observations have implications for the supposed origination of this group, based on molecular divergence estimates.  相似文献   

On the performance of the new NWP nowcasting system at the Danish Meteorological Institute during a heavy rain period     

Bjarke Tobias Olsen  Ulrik Smith Korsholm  Claus Petersen  Niels Woetmann Nielsen  Bent Hansen Sass  Henrik Vedel 《Meteorology and Atmospheric Physics》2015,127(5):519-535

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Oxygen and carbon isotope ratios in the martian atmosphere     

Vladimir A. Krasnopolsky  Jean Pierre Maillard  Tobias C. Owen  Robert A. Toth  Michael D. Smith 《Icarus》2007,192(2):396-403

Oxygen and carbon isotope ratios in the martian CO₂ are key values to study evolution of volatiles on Mars. The major problems in spectroscopic determinations of these ratios on Mars are uncertainties associated with: (1) equivalent widths of the observed absorption lines, (2) line strengths in spectroscopic databases, and (3) thermal structure of the martian atmosphere during the observation. We have made special efforts to reduce all these uncertainties. We observed Mars using the Fourier Transform Spectrometer at the Canada–France–Hawaii Telescope. While the oxygen and carbon isotope ratios on Mars were byproducts in the previous observations, our observation was specifically aimed at these isotope ratios. We covered a range of 6022 to 6308 cm⁻¹ with the highest resolving power of ν/δν=3.5×10⁵ and a signal-to-noise ratio of 180 in the middle of the spectrum. The chosen spectral range involves 475 lines of the main isotope, 184 lines of ¹³CO₂, 181 lines of CO¹⁸O, and 119 lines of CO¹⁷O. (Lines with strengths exceeding 10⁻²⁷ cm at 218 K are considered here.) Due to the high spectral resolution, most of the lines are not blended. Uncertainties of retrieved isotope abundances are in inverse proportion to resolving power, signal-to-noise ratio, and square root of the number of lines. Laboratory studies of the CO₂ isotope spectra in the range of our observation achieved an accuracy of 1% in the line strengths. Detailed observations of temperature profiles using MGS/TES and data on temperature variations with local time from two GCMs are used to simulate each absorption line at various heights in each part of the instrument field of view and then sum up the results. Thermal radiation of Mars' surface and atmosphere is negligible in the chosen spectral range, and this reduces errors associated with uncertainties in the thermal structure on Mars. Using a combination of all these factors, the highest accuracy has been achieved in measuring the CO₂ isotope ratios: ¹³C/¹²C = 0.978 ± 0.020 and ¹⁸O/¹⁶O = 1.018 ± 0.018 times the terrestrial standards. Heavy isotopes in the atmosphere are enriched by nonthermal escape and sputtering, and depleted by fractionation with solid-phase reservoirs. The retrieved ratios show that isotope fractionation between CO₂ and oxygen and carbon reservoirs in the solid phase is almost balanced by nonthermal escape and sputtering of O and C from Mars.  相似文献   

Improving the simulation of fine-resolution landscape changes by coupling top-down and bottom-up land use and cover changes rules     

Thomas Houet  Noémie Schaller  Mathieu Castets  Cédric Gaucherel 《International journal of geographical information science》2014,28(9):1848-1876

Modelling land use and cover changes (LUCC) at local and landscape scales simultaneously, in terms of composition and configuration, remains today highly challenging. Agricultural landscapes offer an illustrative context for this purpose. This article presents a modelling platform (DYPAL) able to simulate LUCC at both local (agricultural parcel, farm) and landscape levels by combining LUCC processes with an optimization algorithm. The efficiency of this approach is assessed by comparing it with an approach applying the same LUCC processes without optimization. Simulations have been developed for two representative case studies of temperate intensive agricultural mosaics: (1) neutral landscapes with simple and theoretical rules and (2) observed landscapes with realistic crop successions rules. Results show that this modelling platform improves the simulation of LUCC achieved at fine resolution, although not systematically. Improvements are observed when compared to theoretical farming practices. But, when compared with an observed landscape, it is true for one type of (arable) farms only. Several hypotheses are discussed, such as the fact that farmers possibly do not follow optimized rules. Finally, this study illustrates that the use of several indices is crucial to assess whether a simulated landscape is realistic or not, because it does not rely to the assessment of the predictive power of the model.  相似文献   

Turbulent flux observations and modelling over a shallow lake and a wet grassland in the Nam Co basin,Tibetan Plateau   总被引：2，自引：1，他引：1  

Tobias?BiermannEmail author  Wolfgang?Babel  Weiqiang?Ma  Xuelong?Chen  Elisabeth?Thiem  Yaoming?Ma  Thomas?Foken 《Theoretical and Applied Climatology》2014,116(1-2):301-316

The Tibetan Plateau plays an important role in the global water cycle and is strongly influenced by climate change. While energy and matter fluxes have been more intensely studied over land surfaces, a large proportion of lakes have either been neglected or parameterised with simple bulk approaches. Therefore, turbulent fluxes were measured over wet grassland and a shallow lake with a single eddy-covariance complex at the shoreline in the Nam Co basin in summer 2009. Footprint analysis was used to split observations according to the underlying surface, and two sophisticated surface models were utilised to derive gap-free time series. Results were then compared with observations and simulations from a nearby eddy-covariance station over dry grassland, yielding pronounced differences. Observations and footprint integrated simulations compared well, even for situations with flux contributions including grassland and lake. The accessibility problem for EC measurements on lakes can be overcome by combining standard meteorological measurements at the shoreline with model simulations, only requiring representative estimates of lake surface temperature.  相似文献   

Response of the Atlantic meridional overturning circulation to a reversal of greenhouse gas increases     

L. C. Jackson  N. Schaller  R. S. Smith  M. D. Palmer  M. Vellinga 《Climate Dynamics》2014,42(11-12):3323-3336

The reversibility of the Atlantic meridional overturning circulation (AMOC) is investigated in multi-model experiments using global climate models (GCMs) where CO₂ concentrations are increased by 1 or 2 % per annum to 2× or 4× preindustrial conditions. After a period of stabilisation the CO₂ is decreased back to preindustrial conditions. In most experiments when the CO₂ decreases, the AMOC recovers before becoming anomalously strong. This "overshoot" is up to an extra 18.2Sv or 104 % of its preindustrial strength, and the period with an anomalously strong AMOC can last for several hundred years. The magnitude of this overshoot is shown to be related to the build up of salinity in the subtropical Atlantic during the previous period of high CO₂ levels. The magnitude of this build up is partly related to anthropogenic changes in the hydrological cycle. The mechanisms linking the subtropical salinity increase to the subsequent overshoot are analysed, supporting the relationship found. This understanding is used to explain differences seen in some models and scenarios. In one experiment there is no overshoot because there is little salinity build up, partly as a result of model differences in the hydrological cycle response to increased CO₂ levels and partly because of a less aggressive scenario. Another experiment has a delayed overshoot, possibly as a result of a very weak AMOC in that GCM when CO₂ is high. This study identifies aspects of overshoot behaviour that are robust across a multi-model and multi-scenario ensemble, and those that differ between experiments. These results could inform an assessment of the real-world AMOC response to decreasing CO₂.  相似文献