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  • 1
    Publication Date: 2008-12-05
    Description: Terrestrial wetland emissions are the largest single source of the greenhouse gas methane. Northern high-latitude wetlands contribute significantly to the overall methane emissions from wetlands, but the relative source distribution between tropical and high-latitude wetlands remains uncertain. As a result, not all the observed spatial and seasonal patterns of atmospheric methane concentrations can be satisfactorily explained, particularly for high northern latitudes. For example, a late-autumn shoulder is consistently observed in the seasonal cycles of atmospheric methane at high-latitude sites, but the sources responsible for these increased methane concentrations remain uncertain. Here we report a data set that extends hourly methane flux measurements from a high Arctic setting into the late autumn and early winter, during the onset of soil freezing. We find that emissions fall to a low steady level after the growing season but then increase significantly during the freeze-in period. The integral of emissions during the freeze-in period is approximately equal to the amount of methane emitted during the entire summer season. Three-dimensional atmospheric chemistry and transport model simulations of global atmospheric methane concentrations indicate that the observed early winter emission burst improves the agreement between the simulated seasonal cycle and atmospheric data from latitudes north of 60 degrees N. Our findings suggest that permafrost-associated freeze-in bursts of methane emissions from tundra regions could be an important and so far unrecognized component of the seasonal distribution of methane emissions from high latitudes.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Mastepanov, Mikhail -- Sigsgaard, Charlotte -- Dlugokencky, Edward J -- Houweling, Sander -- Strom, Lena -- Tamstorf, Mikkel P -- Christensen, Torben R -- England -- Nature. 2008 Dec 4;456(7222):628-30. doi: 10.1038/nature07464.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉GeoBiosphere Science Centre, Physical Geography and Ecosystems Analysis, Lund University, Solvegatan 12, 22362, Lund, Sweden.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/19052625" target="_blank"〉PubMed〈/a〉
    Keywords: Arctic Regions ; Atmosphere/*chemistry ; Cold Climate ; *Freezing ; Greenland ; Methane/analysis/*metabolism ; Seasons ; Soil/analysis ; *Wetlands
    Print ISSN: 0028-0836
    Electronic ISSN: 1476-4687
    Topics: Biology , Chemistry and Pharmacology , Medicine , Natural Sciences in General , Physics
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  • 2
  • 3
    Publication Date: 2008-07-15
    Description: Satellite observations of methane (CH4) using the Atmospheric Infrared Sounder (AIRS) on the EOS/Aqua platform from 2003–2007 demonstrate a strong, plume-like enhancement of CH4 in the middle to upper troposphere over the South Asia during July, August and September, and its maximum occurs in early September. Simulations using the global tracer model version 3 (TM3) also show similar seasonal enhancement of CH4 in the same region. The model results also suggest that this enhancement is associated with transport process and local surface emissions, thus the observations to tropospheric CH4during the monsoon season may be used to constrain the models for a better estimation of Asian CH4 sources. Further comparisons between AIRS observations and the model simulations indicate a possible overestimate of CH4 emissions from rice paddies in Southeast Asia. Moreover, the observed tropospheric CH4 enhancement from AIRS provides evidence for the strong transport of atmospheric pollutants from the lower to the upper troposphere in Asia during the monsoon season, and the observed rapid disappearance of local CH4 maximum in September may provide valuable information for studying the dissipation of the Tibetan anticyclone and the withdrawal of monsoon.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 4
    Publication Date: 2009-03-20
    Description: Inverse modeling techniques used to quantify surface carbon fluxes commonly assume that the uncertainty of fossil fuel CO2 (FFCO2) emissions is negligible and that intra-annual variations can be neglected. To investigate these assumptions, we analyzed the differences between four fossil fuel emission maps with spatial and temporal differences over Europe and their impact on the model simulated CO2 concentration. Large temporal flux variations characterize the hourly fields (~40% and ~80% for the seasonal and diurnal cycles, peak-to-peak) and annual country totals differ by 10% on average and up to 40% for some countries (i.e., The Netherlands). These emissions have been prescribed to seven different transport models, resulting in 28 different FFCO2 concentrations fields. The modeled FFCO2 concentration time series at surface sites using time-varying emissions show larger seasonal cycles (+2 ppm at the Hungarian tall tower (HUN)) and smaller diurnal cycles in summer (−1 ppm at HUN) than when using constant emissions. The concentration range spanned by all simulations varies between stations, and is generally larger in winter (up to ~10 ppm peak-to-peak at HUN) than in summer (~5 ppm). The contribution of transport model differences to the simulated concentration std-dev is 2–3 times larger than the contribution of emission differences only, at typical European sites used in global inversions. These contributions to the hourly (monthly) std-dev's amount to ~1.2 (0.8) ppm and ~0.4 (0.3) ppm for transport and emissions, respectively. First comparisons of the modeled concentrations with 14C-based fossil fuel CO2 observations show that the large transport differences still hamper a quantitative evaluation/validation of the emission inventories. Changes in the estimated monthly biosphere flux (Fbio) over Europe, using two inverse modeling approaches, are relatively small (less that 5%) while changes in annual Fbio (up to ~0.15 Gt C/yr) are only slightly smaller than the differences in annual emission totals and around 30% of the mean European ecosystem carbon sink. These results point to an urgent need to improve not only the transport models but also the assumed spatial and temporal distribution of fossil fuel emission maps.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 5
    Publication Date: 2005-11-08
    Description: SCIAMACHY CO2 measurements show a large variability in total column CO2 over the Sahara desert of up to 10%, which is not anticipated from in situ measurements and cannot be explained by results of atmospheric models. Comparisons with colocated aerosol measurements by TOMS and MISR over the Sahara indicate that the seasonal variation of SCIAMACHY-observed CO2 strongly resembles seasonal variations of windblown dust. Correlation coefficients of monthly datasets of colocated MISR aerosol optical depth and SCIAMACHY CO2 vary between 0.6 and 0.8, indicating that about half of the CO2 variance is explained by aerosol optical depth. Radiative transfer model calculations confirm the role of dust and can explain the size of the errors. Sensitivity tests suggest that the remaining variance may largely be explained by variations in the vertical distribution of dust. Further calculations for a few typical aerosol classes and a broad range of atmospheric conditions show that the impact of aerosols on SCIAMACHY retrieved CO2 is by far the largest over the Sahara, but may also reach significant levels elsewhere. Over the continents, aerosols lead mostly to overestimated CO2 columns with the exception of biomass burning plumes and dark coniferous forests. Inverse modelling calculations confirm that aerosol correction of SCIAMACHY CO2 measurements is needed to derive meaningful source and sink estimates. Methods for correcting aerosol-induced errors exist, but so far mainly on the basis of theoretical considerations. As demonstrated by this study, SCIAMACHY may contribute to a verification of such methods using real data.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 6
    Publication Date: 2005-02-10
    Description: This paper describes the global chemistry Transport Model, version 5 (TM5) which allows two-way nested zooming. The model is used for global studies which require high resolution regionally but can work on a coarser resolution globally. The zoom algorithm introduces refinement in both space and time in some predefined regions. Boundary conditions of the zoom region are provided by a coarser parent grid and the results of the zoom area are communicated back to the parent. A case study using 222Rn measurements that were taken during the MINOS campaign reveals the advantages of local zooming. As a next step, it is investigated to what extent simulated concentrations over Europe are influenced by using an additional zoom domain over North America. An artificial ozone-like tracer is introduced with a lifetime of twenty days and simplified non-linear chemistry. The concentration differences at Mace Head (Ireland) are generally smaller than 10%, much smaller than the effects of the resolution enhancement over Europe. Thus, coarsening of resolution at some distance of a sampling station seems allowed. However, it is also noted that the budgets of the tracers change considerably due to resolution dependencies of, for instance, vertical transport. Due to the two-way nested algorithm, TM5 offers a consistent tool to study the effects of grid refinement on global atmospheric chemistry issues like intercontinental transport of air pollution.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 7
    Publication Date: 2008-08-29
    Description: The possible use of 14CO measurements to constrain hydroxyl radical (OH) concentrations in the atmosphere is investigated. 14CO is mainly produced in the upper atmosphere from cosmic radiation. Measurements of 14CO at the surface show lower concentrations compared to the upper atmospheric source region, which is the result of oxidation by OH. In this paper, the sensitivity of 14CO mixing ratio surface measurements to the 3-D OH distribution is assessed with the TM5 model. Simulated 14CO mixing ratios agree within a few molecules 14CO cm−3 (STP) with existing measurements at five locations worldwide. The simulated cosmogenic 14CO distribution appears mainly sensitive to the assumed upper atmospheric 14C source function, and to a lesser extend to model resolution. As a next step, the sensitivity of 14CO measurements to OH is calculated with the adjoint TM5 model. The results indicate that 14CO measurements taken in the tropics are sensitive to OH in a spatially confined region that varies strongly over time due to meteorological variability. Given measurements with an accuracy of 0.5 molecules 14CO cm−3 STP, a good characterization of the cosmogenic 14CO fraction, and assuming perfect transport modeling, a single 14CO measurement may constrain OH to 0.2–0.3×106 molecules OH cm−3 on time scales of 6 months and spatial scales of 70×70 degrees (latitude×longitude) between the surface and 500 hPa. The sensitivity of 14CO measurements to high latitude OH is about a factor of five higher. This is in contrast with methyl chloroform (MCF) measurements, which show the highest sensitivity to tropical OH, mainly due to the temperature dependent rate constant of the MCF–OH reaction. A logical next step will be the analysis of existing 14CO measurements in an inverse modeling framework. This paper presents the required mathematical framework for such an analysis.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
    Publication Date: 2005-01-01
    Print ISSN: 0273-1177
    Electronic ISSN: 1879-1948
    Topics: Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Published by Elsevier
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  • 9
    Publication Date: 2007-07-19
    Description: The possible use of 14CO measurements to constrain hydroxyl radical (OH) concentrations in the atmosphere is investigated.14CO is mainly produced in the upper atmosphere from cosmic radiation. During transport to measurement locations at the Earth's surface 14CO is oxidized by OH. In this paper, the sensitivity of 14CO mixing ratio measurements to the 3-D OH distribution is assessed with the TM5 model. Simulated 14CO mixing ratios compare reasonably well with atmospheric measurements taken at five locations worldwide. As a next step, the sensitivity of 14CO measurements to OH is calculated with the adjoint TM5 model. For our sensitivity calculations the adjoint methodology outlined in the paper offers computational advantages compared to forward model calculations. The results indicate that 14CO measurements, especially those taken in the tropics, are sensitive to OH in a spatially confined region. Moreover, the OH sensitivity at a certain location varies strongly over time due to meteorological variability. On average, 14CO measurements are about 5 times more sensitive to OH at high latitudes than to OH in the tropics. Moreover, the measurements are sensitive to OH in the main 14CO source region in the upper atmosphere. It will therefore be difficult to assign model-measurement discrepancies to either the 14CO source uncertainty or to the OH sink. Nevertheless, the large distance between the 14CO source region and the measurement locations should allow the retrieval of information on OH. Specifically, the sensitivity to OH in the lower atmosphere during a relatively short time span may offer the possibility to constrain local OH. These efforts will strongly depend on the number of measurements available and on our ability to accurately model the 14CO transport.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 10
    Publication Date: 2005-05-25
    Description: SCIAMACHY CO2 measurements show a large variability in total column CO2 over the Sahara desert of up to 10% that is not anticipated from in situ measurements and cannot be explained by results of atmospheric models. Comparisons with colocated aerosol measurements by TOMS and MISR over the Sahara indicate that the seasonal variation of SCIAMACHY-observed CO2 strongly resembles seasonal variations of windblown dust. Correlation coefficients of monthly datasets of colocated MISR aerosol optical depth and SCIAMACHY CO2 vary between 0.6 and 0.8, indicating that about half of the CO2 variance is explained by aerosol optical depth. Radiative transfer model calculations confirm the role of dust and can explain the size of the errors. Sensitivity tests suggest that the remaining variance may largely be explained by variations in the vertical distribution of dust. Further calculations for a few typical aerosol classes and a broad range of atmospheric conditions show that the impact of aerosols on SCIAMACHY retrieved CO2 is by far the largest over the Sahara, but may also reach significant levels elsewhere. Inverse modelling calculations indicate that continental scale source and sink estimation on the basis of SCIAMACHY CO2 data without aerosol correction leads to significant errors. To improve terrestrial CO2 flux estimates by inverse modelling using SCIAMACHY measurements at 1.6μm, aerosol correction will be needed. Methods for correcting aerosol-induced errors exist, but so far mainly on the basis of theoretical considerations. As demonstrated by this study, SCIAMACHY may contribute to a verification of such methods using real data.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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