Douglas E. J. Worthy

An atmospheric perspective on North American carbon dioxide exchange: CarbonTracker

We present an estimate of net CO2 exchange between the terrestrial biosphere and the atmosphere across North America for every week in the period 2000 through 2005. This estimate is derived from a set of 28,000 CO2 mole fraction observations in the global atmosphere that are fed into a state-of-the-art data assimilation system for CO2 called CarbonTracker. By design, the surface fluxes produced in CarbonTracker are consistent with the recent history of CO2 in the atmosphere and provide constraints on the net carbon flux independent from national inventories derived from accounting efforts. We find the North American terrestrial biosphere to have absorbed −0.65 PgC/yr (1 petagram = 1015 g; negative signs are used for carbon sinks) averaged over the period studied, partly offsetting the estimated 1.85 PgC/yr release by fossil fuel burning and cement manufacturing. Uncertainty on this estimate is derived from a set of sensitivity experiments and places the sink within a range of −0.4 to −1.0 PgC/yr. The estimated sink is located mainly in the deciduous forests along the East Coast (32%) and the boreal coniferous forests (22%). Terrestrial uptake fell to −0.32 PgC/yr during the large-scale drought of 2002, suggesting sensitivity of the contemporary carbon sinks to climate extremes. CarbonTracker results are in excellent agreement with a wide collection of carbon inventories that form the basis of the first North American State of the Carbon Cycle Report (SOCCR), to be released in 2007. All CarbonTracker results are freely available at http://carbontracker.noaa.gov.

CO2 surface fluxes at grid point scale estimated from a global 21 year reanalysis of atmospheric measurements

This paper documents a global Bayesian variational inversion of CO2 surface fluxes during the period 1988-2008. Weekly fluxes are estimated on a 3.75 degrees x 2.5 degrees (longitude-latitude) grid throughout the 21 years. The assimilated observations include 128 station records from three large data sets of surface CO2 mixing ratio measurements. A Monte Carlo approach rigorously quantifies the theoretical uncertainty of the inverted fluxes at various space and time scales, which is particularly important for proper interpretation of the inverted fluxes. Fluxes are evaluated indirectly against two independent CO2 vertical profile data sets constructed from aircraft measurements in the boundary layer and in the free troposphere. The skill of the inversion is evaluated by the improvement brought over a simple benchmark flux estimation based on the observed atmospheric growth rate. Our error analysis indicates that the carbon budget from the inversion should be more accurate than the a priori carbon budget by 20% to 60% for terrestrial fluxes aggregated at the scale of subcontinental regions in the Northern Hemisphere and over a year, but the inversion cannot clearly distinguish between the regional carbon budgets within a continent. On the basis of the independent observations, the inversion is seen to improve the fluxes compared to the benchmark: the atmospheric simulation of CO2 with the Bayesian inversion method is better by about 1 ppm than the benchmark in the free troposphere, despite possible systematic transport errors. The inversion achieves this improvement by changing the regional fluxes over land at the seasonal and at the interannual time scales. (Less)

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.

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.

Rising atmospheric methane: 2007-2014 growth and isotopic shift

From 2007 to 2013, the globally averaged mole fraction of methane in the atmosphere increased by 5.7 ± 1.2 ppb yr−1. Simultaneously, δ13CCH4 (a measure of the 13C/12C isotope ratio in methane) has shifted to significantly more negative values since 2007. Growth was extreme in 2014, at 12.5 ± 0.4 ppb, with a further shift to more negative values being observed at most latitudes. The isotopic evidence presented here suggests that the methane rise was dominated by significant increases in biogenic methane emissions, particularly in the tropics, for example, from expansion of tropical wetlands in years with strongly positive rainfall anomalies or emissions from increased agricultural sources such as ruminants and rice paddies. Changes in the removal rate of methane by the OH radical have not been seen in other tracers of atmospheric chemistry and do not appear to explain short-term variations in methane. Fossil fuel emissions may also have grown, but the sustained shift to more 13C-depleted values and its significant interannual variability, and the tropical and Southern Hemisphere loci of post-2007 growth, both indicate that fossil fuel emissions have not been the dominant factor driving the increase. A major cause of increased tropical wetland and tropical agricultural methane emissions, the likely major contributors to growth, may be their responses to meteorological change.

Isotope analysis based source identification for atmospheric CH4 and CO sampled across Russia using the Trans‐Siberian railroad

The isotopic composition of carbon monoxide (13C, 14C, 18O) and methane (13C, D) was measured on air samples collected between Vladivostok and Moscow using the Trans-Siberian railroad during August 1996. Apart from short term fluctuations in the direct vicinity of sources, continuous measurements of CO and CH4 showed sustained, elevated mixing ratios over several hundreds of kilometers indicating the large scale influencing of traversed air masses by significant sources. Persistent, enhanced CH4 levels were found over the west Siberian lowlands concurrent with significantly depleted δ13C and δD values. The derived isotopic signature of the CH4 source (δ13C = −62.5±4.7‰ V-PDB; δD = −311±14‰ V-SMOW) clearly indicates the dominance of biogenic CH4, with the west Siberian wetlands being the most likely candidate. A second major feature in the data set is the enormous enhancement of CO (up to 1500 nmol/mol) east of Chita, extending over a 2000 km section along the river Amur. The 14CO measurements and back trajectory analyses identify biomass burning as the origin of the highly elevated CO. This is further supported by the δ18O(CO) and the δ13C/δD signature of the accompanying moderate CH4 enhancement.

Analysis of long‐range transport events at Alert, Northwest Territories, during the Polar Sunrise Experiment

In situ measurements of carbon dioxide, methane, black carbon, peroxyacetylnitrate, condensation nuclei, and radon were made from the Canadian Baseline Atmospheric Monitoring Observatory at Alert, Northwest Territories, Canada (82°28′N, 62°30′W′) during the “Polar Sunrise Experiment” (January 16 to April 20, 1992). The time series of methane, carbon dioxide, peroxyacetylnitrate, and black carbon were frequently highly correlated during January and February during well-defined episodes lasting from 2 to 5 days. This is consistent with data from earlier years. Shortly after polar sunrise, the temporal variability in both trace gases and aerosols diminished. Using a definition of black carbon concentrations exceeding 100 ng m−3, 11 long-range transport episodes were defined. Lagrangian 5-day back trajectories along with the concentration data were classified into six geographical sectors to characterize the major episodes. The winter variability is related to synoptic meteorology, weak vertical mixing, and rapid air mass transport originating from Siberian and/or European source regions. Measurements of the radon daughter (222Rn) activity in the atmosphere were used to further explore the transport of continental material across the Arctic basin.

Western European N2O emissions: A top‐down approach based on atmospheric observations

We present a 3 year record of continuous gas chromatographic nitrous oxide (N2O) observations performed at the urban station Heidelberg (Germany) together with weekly flask data from a remote continental site, Schauinsland (Black Forest, Germany), and two-weekly integrated data from the maritime background station Izana (Canary Islands). These data are supplemented by continuous atmospheric radon 222 observations. Mean rates of increase of N2O of 0.70–0.78 ppb yr−1 were observed over the continent and in maritime background air (Izana). The well-mixed continental mixing ratio was found to be higher by only 1.1 ppb (Schauinsland) and 2.4 ppb (Heidelberg) than for maritime background air. Specially tailored data selection of the Heidelberg record allowed the changing influence of a regional N2O point source (adipic acid production, BASF AG) to be clearly identified. The radon (222Rn) tracer method was applied to nighttime N2O observations at Heidelberg to estimate mean regional emissions, which changed from (161 ± 32) μg N2O-N m−2 h−1 in 1996–1997 to (77 ± 10) μg N2O-N m−2 h−1 in 1998 as a consequence of 90% emission reduction from BASF. An estimate of the continental N2O flux from southwestern Europe based on further selected Heidelberg data (only well-mixed, late afternoon situations) and observations from the Schauinsland station yielded mean N2O fluxes of (43 ± 5) μg N2O-N m−2 h−1 and (42 ± 4) μg N2O-N m−2 h−1. These results compare well with statistical emissions inventories, when taking into account possible systematic errors of the radon tracer method of 30–35%.

Global CO2 fluxes inferred from surface air-sample measurements and from TCCON retrievals of the CO2 total column

We present the first estimate of the global distribution of CO_2 surface fluxes from 14 stations of the Total Carbon Column Observing Network (TCCON). The evaluation of this inversion is based on 1) comparison with the fluxes from a classical inversion of surface air-sample-measurements, and 2) comparison of CO_2 mixing ratios calculated from the inverted fluxes with independent aircraft measurements made during the two years analyzed here, 2009 and 2010. The former test shows similar seasonal cycles in the northern hemisphere and consistent regional carbon budgets between inversions from the two datasets, even though the TCCON inversion appears to be less precise than the classical inversion. The latter test confirms that the TCCON inversion has improved the quality (i.e., reduced the uncertainty) of the surface fluxes compared to the assumed or prior fluxes. The consistency between the surface-air-sample-based and the TCCON-based inversions despite remaining flaws in transport models opens the possibility of increased accuracy and robustness of flux inversions based on the combination of both data sources and confirms the usefulness of space-borne monitoring of the CO_2 column.

Regional source/sink impact on the diurnal, seasonal and inter-annual variations in atmospheric CO2 at a boreal forest site in Canada

Time series of in-situ CO2 data from Fraserdale (50°N, 81°W) in the northern Ontario boreal forest is described, together with an analysis of observed variations occurring on daily to interannual timescales. Atmospheric CO2 measurements at Fraserdale reflect a complex interaction between the daily cycle of the vegetative carbon flux and the daily evolution of the boundary layer mixing dynamics. This is particularly evident during the growing season, when CO2 concentrations are influenced strongly by local and regional biospheric activities. In addition, the atmospheric CO2 measurements at Fraserdale are greatly influenced by the direction of atmospheric transport, and reflect the complex heterogeneous distribution of ecosystem types around the site. Averaged over the 7-yr period from 1990 to 1996, the seasonal cycle associated with air from west and northwest of the site shows an amplitude of ~19 ppm, while that associated with air from the south and southwest shows an amplitude of ~23 ppm; the seasonal minimum, on average, occurs about a week earlier in the latter case than in the former. This is reflective of the fact that many of the deciduous trees are located to the south and southwest of Fraserdale. Furthermore, its location in the boreal forest causes the seasonal minimum to occur on average in early August at Fraserdale, compared to late August observed at Alert and at many other background stations in the high-latitude Northern Hemisphere. At the Fraserdale site there is no statistically significant indication, during the 1990–1996 study period, of changes in the length of the growing season (as measured by zero crossing points in the seasonal cycle).