Ingeborg Levin

The tropospheric 14CO2 level in mid latitudes of the Northern Hemisphere (1959-2003)

A comprehensive tropospheric (super 14) CO (sub 2) data set of quasi-continuous observations covering the time span from 1959 to 2003 is presented. Samples were collected at 3 European mountain sites at height levels of 1205 m (Schauinsland), 1800 m (Vermunt), and 3450 m asl (Jungfraujoch), and analyzed in the Heidelberg Radiocarbon Laboratory. The data set from Jungfraujoch (1986-2003) is considered to represent the free tropospheric background level at mid-latitudes of the Northern Hemisphere, as it compares well with recent (yet unpublished) measurements made at the marine baseline station Mace Head (west coast of Ireland). The Vermunt and Schauinsland records are significantly influenced by regional European fossil fuel CO (sub 2) emissions. The respective delta (super 14) CO (sub 2) depletions, on an annual mean basis, are, however, only 5 ppm less than at Jungfraujoch. Vermunt and Schauinsland both represent the mean continental European troposphere.

Inverse modeling of global and regional CH4 emissions using SCIAMACHY satellite retrievals

Methane retrievals from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) instrument onboard ENVISAT provide important information on atmospheric CH_4 sources, particularly in tropical regions which are poorly monitored by in situ surface observations. Recently, Frankenberg et al. (2008a, 2008b) reported a major revision of SCIAMACHY retrievals due to an update of spectroscopic parameters of water vapor and CH_4. Here, we analyze the impact of this revision on global and regional CH_4 emissions estimates in 2004, using the TM5-4DVAR inverse modeling system. Inversions based on the revised SCIAMACHY retrievals yield ∼20% lower tropical emissions compared to the previous retrievals. The new retrievals improve significantly the consistency between observed and assimilated column average mixing ratios and the agreement with independent validation data. Furthermore, the considerable latitudinal and seasonal bias correction of the previous SCIAMACHY retrievals, derived in the TM5-4DVAR system by simultaneously assimilating high-accuracy surface measurements, is reduced by a factor of ∼3. The inversions result in significant changes in the spatial patterns of emissions and their seasonality compared to the bottom-up inventories. Sensitivity tests were done to analyze the robustness of retrieved emissions, revealing some dependence on the applied a priori emission inventories and OH fields. Furthermore, we performed a detailed validation of simulated CH_4 mixing ratios using NOAA ship and aircraft profile samples, as well as stratospheric balloon samples, showing overall good agreement. We use the new SCIAMACHY retrievals for a regional analysis of CH_4 emissions from South America, Africa, and Asia, exploiting the zooming capability of the TM5 model. This allows a more detailed analysis of spatial emission patterns and better comparison with aircraft profiles and independent regional emission estimates available for South America. Large CH_4 emissions are attributed to various wetland regions in tropical South America and Africa, seasonally varying and opposite in phase with CH_4 emissions from biomass burning. India, China and South East Asia are characterized by pronounced emissions from rice paddies peaking in the third quarter of the year, in addition to further anthropogenic emissions throughout the year.

Soil texture parameterization of the methane uptake in aerated soils

Long-term records of the methane uptake by five different aerated soils in South-West Germany and spot measurements in Western Europe, North America, and North-West Africa are presented. A good correlation between the methane uptake rate and soil permeability, obtained from parallel 222Radon flux and concentration measurements of methane and 222Radon in soil air indicates, that methane consumption in aerated soils is mainly controlled by the gas transport resistance within the soil. Soil temperature is found to be of minor influence on the methane flux from the atmosphere into the soil. The soils investigated were classified with respect to the three major soil texture classes - coarse, medium, and fine - representing soils with low, medium, and high gas transport resistance, respectively. Average methane uptake rates for each soil texture class were determined and extrapolated to fit into the scheme of the NASA-GISS global digital data set of soil types (Staub et al., 1987). Assuming that the observed relation between methane uptake rate and soil permeability (soil texture) is valid for all kinds of aerated soils, methane uptake rates are estimated on a regional and global scale. From this parameterization we calculate a global CH4 soil sink in the range of 9.0 to 55.9 Tg CH4/a with a best estimate of 28.7 Tg CH4/a. This corresponds to about 7% of the total global destruction rate by OH radicals.

Observations and modelling of the global distribution and long-term trend of atmospheric 14CO2.

Global high-precision atmospheric Δ14CO2 records covering the last two decades are presented, and evaluated in terms of changing (radio)carbon sources and sinks, using the coarse-grid carbon cycle model GRACE. Dedicated simulations of global trends and interhemispheric differences with respect to atmospheric CO2 as well as δ13CO2 and Δ14CO2, are shown to be in good agreement with the available observations (1940–2008). While until the 1990s the decreasing trend of Δ14CO2 was governed by equilibration of the atmospheric bomb 14C perturbation with the oceans and terrestrial biosphere, the largest perturbation today are emissions of 14C-free fossil fuel CO2. This source presently depletes global atmospheric Δ14CO2 by 12–14‰ yr−1, which is partially compensated by 14CO2 release from the biosphere, industrial 14C emissions and natural 14C production. Fossil fuel emissions also drive the changing north–south gradient, showing lower Δ14C in the northern hemisphere only since 2002. The fossil fuel-induced north–south (and also troposphere–stratosphere) Δ14CO2 gradient today also drives the tropospheric Δ14CO2 seasonality through variations of air mass exchange between these atmospheric compartments. Neither the observed temporal trend nor the Δ14CO2 north–south gradient may constrain global fossil fuel CO2 emissions to better than 25%, due to large uncertainties in other components of the (radio)carbon cycle.

Twenty years of atmospheric 14CO2 observations at Schauinsland Station, Germany

We present and discuss quasi-continuous long-term 14C02 observations from the continental background station Schauinsland (48°N, 8°E, 1205 m asl, Black Forest, southern Germany). The observed steady decline of atmospheric 14002 from 1977 to 1996 can be described by a single exponential function with an e-folding time of (16.3 ± 0.2) yr. Summer means (May to August) in atmospheric 14C02 at Schauinsland compare within ∆4C = ±4‰ with measurements made on individual rings from a tree grown in the near vicinity of the Schauinsland site. Both data sets are slightly depleted by up to 5‰ if compared to maritime background measurements of atmospheric 14C02 made at Izana, Tenerife. This is due to the influence of fossil fuel CO2 emissions over the European continent as well as generally in mid latitudes of the Northern Hemisphere. δ13C analyses from the Schauinsland samples show mean seasonal variations with an amplitude of ±0.4‰, caused by atmosphere-biosphere exchange, and a mean decrease from 1977 to 1996 of δ13C = -0.017‰ yr. This trend is mainly due to an increasing quantity of fossil fuel CO2 in the atmosphere, depleted in 13C/12C ratio, and compares well to trends measured at other stations in mid-to-high northern latitudes.

Sulfur hexafluoride—A powerful new atmospheric tracer

Long-term observations of the atmospheric trace gas sulfur hexafluoride (SF6) at four background monitoring stations, Neumayer, Antarctica (1986–1994), Cape Grim, Tasmania (1978–1994), Izafna, Canary Islands (1991–1994) and Alert, Canada (1993–1994) are presented. These data sets are supplemented by two meridional profiles collected over the Atlantic Ocean (1990 and 1993) and occasional observations at the regional site Fraserdale, Canada (1994). The analytical system and the method of SF6 calibration are described. Compared with data from Neumayer and Izafia reported earlier, measurements are updated for all sites until the end of 1994 and the precision has improved by more than a factor of 2. With the Cape Grim archived air samples, the atmospheric SF6 chronology is extended by 8 more years back to 1978. For the period from January 1978 to December 1994 the data confirm a stable and unbroken quadratic rise in tropospheric SF6 from 0.50 to 3.11 ppt in the southern hemisphere and for July 1991 to December 1994 from 2.69 to 3.44 ppt in the northern hemisphere. The global mean tropospheric increase rate in late 1994 was 0.225 ppt yr−1 (6.9% yr−1). The long term trend and interhemispheric gradients are due to industrial production and emission, rising approximately linearly with time and located predominantly (94%) in the northern hemisphere. The interhemispheric exchange time (1.7 ± 0.2 yr) derived from SF6 ground level observations when using a two-box model of the atmosphere is considerably larger if compared to the exchange time derived from two- and three-dimensional models (1.1 yr). The chemical and biological inertness of SF6 up to stratospheric conditions results in an atmospheric lifetime of more than 800 years and makes SF6 a powerful tool for modelling transport processes in the atmosphere. Moreover, the tropospheric SF6 chronology is a very valuable input function for mixing studies in linked compartments like the stratosphere, the hydrosphere and the cryosphere.

The Effect of Anthropogenic CO2 and 14C Sources on the Distribution of 14C in the Atmosphere

14C measurements on continuous weekly samples of atmospheric CO2 and hydrocarbons, collected in a rather densely populated area are presented. The deviation of the measured 14C data from the clean air level is primarily due to CO2 from the combustion of fossil fuels. This is confirmed by fossil fuel admixture estimates individually calculated with an atmospheric dispersion model. Up to 10 percent admixture is predicted by this model and observed from the 14C shift for weekly averages, particularly during the winter season. Natural CO2 admixture due to soil respiration, however, even in winter, is of the same order of magnitude, but much larger in the warm season: the considerable variations in CO2 concentration in summer are almost exclusively controlled by natural sources. Using tree leaf samples, we have been able to identify boiling water reactors (BWR) as weak sources of 14C02. Atmospheric samples taken in the environment of the pressurized water reactors (PWR) Biblis show that the 14C release of these reactors is primarily in the form of hydrocarbon 14C. The source strength of the various power plants, calculated on the basis of our observations in their environment, ranges from 0.5 to 7Ci per year.

Atmospheric Δ 14 CO 2 trend in Western European background air from 2000 to 2012

ABSTRACT Long-term measurements of atmospheric Δ14CO2 from two monitoring stations, one in the European Alps (Jungfraujoch, Switzerland) and the other in the Black Forest (Schauinsland, Germany), are presented. Both records show a steady decrease, changing from about 6‰ per year at the beginning of the century to only 3‰ per year on average in the last 4 yr. A significant seasonal variation of Δ14CO2 is observed at both sites with maxima during late summer and minima in late winter/early spring. While the Δ14C maxima are similar at Jungfraujoch and Schauinsland, the minima at Schauinsland are lower by up to 10‰, due to a larger influence from 14C-free fossil fuel CO2 emissions in the footprint of the Schauinsland station in winter. Summer mean Δ14C values at Schauinsland are considered best suited as input for studies of biospheric carbon cycling in mid-northern latitudes or for dating of organic material of the last half century.

Verification of German methane emission inventories and their recent changes based on atmospheric observations

Continuous methane concentration records and stable isotope observations measured in the suburbs of Heidelberg, Germany, are presented. While delta13C-CH4 shows a significant trend of -0.14 permil per year, towards more depleted values, no trend is observed in the concentration data. Comparison of the Heidelberg records with clean air observations in the North Atlantic at Izana station (Tenerife) allows the determination of the continental methane excess at Heidelberg, decreasing by 20% from 190 ppb in 1992 to 150 ppb in 1997. The isotope ratio which is associated with this continental methane pile-up in the Heidelberg catchment area shows a significant trend to more depleted values from delta13C (source) = -47.4 ± 1.2 permil in 1992 to 52.9 ± 0.4 permil in 1995/96, pointing to a significant change in the methane source mix. Total methane emissions in the Heidelberg catchment area are estimated using the 222Radon (222Rn) tracer method: from the correlations of half hourly 222Rn and CH4 mixing ratios from 1995 to 1997, and the mean 222Rn exhalation rate from typical soils in the Rhine valley, a mean methane flux of 0.24 ± 0.5 g CH4 km-2 s-1 is derived. For the Heidelberg catchment area with an estimated radius of approximately 150 km, Core Inventories Air 1990 (CORINAIR90) emission estimates yield a flux of 0.47 g CH4 km-2 s-1, which is about 40% higher than the 222Rn derived number if extrapolated to 1990. The discrepancy can be explained by over-estimated emissions from waste management in the CORINAIR90 statistical assessment. The observed decrease in total emissions can be accounted for by decreasing contributions from fossil sources (mainly coal mining) and from cattle breeding. This finding is also supported by the observed decrease in mean source isotopic signatures.

Global increase of SF6 observed in the atmosphere

High precision long-term observations of the trace gas sulphur hexafluoride (SF6) in background air at Neumayer station, Antarctica (1986-1991), and at Izana observatory, Tenerife (1991-1992), are presented. Since the very first measurements in 1970 (0.03pptv), the purely anthropogenic greenhouse gas SF6 has increased by two orders of magnitude to a global mean value of 2.8pptv in 1992. The observations can best be fitted by a quadratic curve with a recent increase rate of 8.3%/yr. A significant north-south gradient of 0.29pptv is observed. From this gradient an interhemispheric exchange time of 1.4 years is derived. A modeled atmospheric budget history agrees reasonably well with estimates of global SF6 production rates and leads to an extrapolated SF6 concentration of about 20pptv for the year 2030.