Posterior Fluxes Research Articles

If Some Critical Regions Achieve Carbon Neutrality, How Will the Global Atmospheric CO2 Concentration Change?

Due to anthropogenic emissions, the global CO2 concentration increases at a rate of approximately 2 ppm per year. With over 130 countries and regions committing to carbon neutrality goals and continuously reducing anthropogenic CO2 emissions, understanding how atmospheric CO2 concentrations will change globally and in other regions has become an intriguing question. Examining different regions’ efforts to reduce anthropogenic CO2 emissions through atmospheric CO2 observations is also meaningful. We used prior and posterior fluxes to drive the TM5 model. The posterior fluxes were based on the China Carbon Monitoring, Verification and Support System for Global (CCMVS-G), which assimilated the atmospheric CO2 concentration data from ground-based observation and satellite observation. We found that the CO2 concentration obtained using the posterior fluxes was more in line with the actual situation. Then, we presented some experiments to estimate how global and regional CO2 concentrations would change if certain key regions and the whole world achieved net zero emissions of anthropogenic CO2. After removing carbon fluxes from China, North America, and Europe, global CO2 concentrations decreased by around 0.58 ppm, 0.22 ppm, and 0.10 ppm, respectively. The most significant decrease occurred in the regions where fluxes were removed, followed by other areas at the same latitude affected by westerly winds. This indicates that fossil fuel flux is the main factor affecting CO2 concentrations, and that meteorological-driven transportation also significantly impacts CO2 concentrations. Most importantly, using this method, it is possible to quantitatively estimate the impact of achieving carbon neutrality in one region on CO2 concentrations in local regions as well as globally.

Invert global and China's terrestrial carbon fluxes over 2019–2021 based on assimilating richer atmospheric CO2 observations

With China's commitment to reach carbon peak by 2030 and achieve carbon neutrality by 2060, it is particularly important to obtain terrestrial ecosystem carbon fluxes with low uncertainty both globally and in China. The use of more observation data may help reduce the uncertainty of inverting carbon fluxes. This study uses the observation data from global stations, background stations and provincial stations in China, as well as the OCO-2 satellite, and uses the China Carbon Monitoring, Verification and Supporting System for Global (CCMVS-G) to estimate the carbon fluxes of global and Chinese terrestrial ecosystems from 2019 to 2021. The results revealed that the global terrestrial ecosystem carbon sink was approximately −3.40 Pg C/yr from 2019 to 2021. The carbon sinks in the Northern Hemisphere are large, especially in Asia, North America, and Europe. From 2019 to 2021, the carbon sink of China's terrestrial ecosystem was approximately −0.44 Pg C/yr. Carbon sinks exhibit significant seasonal and interannual variations in China. After assimilating the observation data, the uncertainty of the posterior flux is smaller than that of the prior flux, a more reasonable distribution of carbon sources and sinks can be obtained, and more accurate boundary conditions can be provided for the China Carbon Monitoring, Verification and Supporting System for Regional (CCMVS-R). In the future, it is important to establish a well-designed CO2 ground-based observation network.

CO2 Flux Inversion With a Regional Joint Data Assimilation System Based on CMAQ, EnKS, and Surface Observations

AbstractMost of China's carbon sink inversion research uses global atmospheric transport models to assimilate natural fluxes, which quantifies the biosphere and ocean carbon budget with a relative coarse spatial resolution and long timescale from a weekly or monthly perspective. Toward high‐resolution inversion of CO2 fluxes, a novel carbon flux forecast model was developed in this study, which was then further used to carry out carbon assimilation based on a regional chemical transport model (CMAQ) at higher spatial (64 × 64 km2) and temporal (1 hr) resolutions. An Ensemble Kalman Smoother was applied as the assimilation algorithm and further extended to assimilate surface CO2 observations. Concentrations and fluxes were simultaneously assimilated as state variables to help reduce the uncertainty in the initial CO2 fields with the joint data assimilation framework (JDAS). In general, the posterior fluxes reproduced the seasonal, daily and hourly variation effectively, demonstrating the ability to fully absorb and utilize observations. Moreover, the influence of the choice of assimilation window on the carbon flux inversion was assessed via sensitivity experiments, revealing 36 hr to be the optimum length. Evaluation of the prior and posterior flux simulations also indicated that JDAS offers reasonable improvements, making it suitable for fine‐scale flux optimization and estimation. In addition, the posterior biosphere estimation in mainland China (−682 TgC yr−1) tends to be the optimal mathematical solution under current sparse observation coverage with daytime photosynthetic uptake, which likely leads to the overestimation of the optimized CO2 sink. This study serves as a basis for future regional and urban assessment.

Modelling the growth of atmospheric nitrous oxide using a global hierarchical inversion

Abstract. Nitrous oxide is a potent greenhouse gas (GHG) and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions, which includes prior emissions with truncated Gaussian distributions and Gaussian model errors, in order to examine the drivers of the atmospheric surface growth rate. We show that both emissions and climatic variability are key drivers of variations in the surface nitrous oxide growth rate between 2011 and 2020. We derive increasing global nitrous oxide emissions, which are mainly driven by emissions between 0 and 30∘ N, with the highest emissions recorded in 2020. Our mean global total emissions for 2011–2020 of 17.2 (16.7–17.7 at the 95 % credible intervals) Tg N yr−1, comprising of 12.0 (11.2–12.8) Tg N yr−1 from land and 5.2 (4.5–5.9) Tg N yr−1 from ocean, agrees well with previous studies, but we find that emissions are poorly constrained for some regions of the world, particularly for the oceans. The prior emissions used in this and other previous work exhibit a seasonal cycle in the extra-tropical Northern Hemisphere that is out of phase with the posterior solution, and there is a substantial zonal redistribution of emissions from the prior to the posterior. Correctly characterizing the uncertainties in the system, for example in the prior emission fields, is crucial for deriving posterior fluxes that are consistent with observations. In this hierarchical inversion, the model-measurement discrepancy and the prior flux uncertainty are informed by the data, rather than solely through “expert judgement”. We show cases where this framework provides different plausible adjustments to the prior fluxes compared to inversions using widely adopted, fixed uncertainty constraints.

The 2019 methane budget and uncertainties at 1° resolution and each country through Bayesian integration Of GOSAT total column methane data and a priori inventory estimates

Abstract. We use optimal estimation (OE) to quantify methane fluxes based on total column CH4 data from the Greenhouse Gases Observing Satellite (GOSAT) and the GEOS-Chem global chemistry transport model. We then project these fluxes to emissions by sector at 1∘ resolution and then to each country using a new Bayesian algorithm that accounts for prior and posterior uncertainties in the methane emissions. These estimates are intended as a pilot dataset for the global stock take in support of the Paris Agreement. However, differences between the emissions reported here and widely used bottom-up inventories should be used as a starting point for further research because of potential systematic errors of these satellite-based emissions estimates. We find that agricultural and waste emissions are ∼ 263 ± 24 Tg CH4 yr−1, anthropogenic fossil emissions are 82 ± 12 Tg CH4 yr−1, and natural wetland/aquatic emissions are 180 ± 10 Tg CH4 yr−1. These estimates are consistent with previous inversions based on GOSAT data and the GEOS-Chem model. In addition, anthropogenic fossil estimates are consistent with those reported to the United Nations Framework Convention on Climate Change (80.4 Tg CH4 yr−1 for 2019). Alternative priors can be easily tested with our new Bayesian approach (also known as prior swapping) to determine their impact on posterior emissions estimates. We use this approach by swapping to priors that include much larger aquatic emissions and fossil emissions (based on isotopic evidence) and find little impact on our posterior fluxes. This indicates that these alternative inventories are inconsistent with our remote sensing estimates and also that the posteriors reported here are due to the observing and flux inversion system and not uncertainties in the prior inventories. We find that total emissions for approximately 57 countries can be resolved with this observing system based on the degrees-of-freedom for signal metric (DOFS > 1.0) that can be calculated with our Bayesian flux estimation approach. Below a DOFS of 0.5, estimates for country total emissions are more weighted to our choice of prior inventories. The top five emitting countries (Brazil, China, India, Russia, USA) emit about half of the global anthropogenic budget, similar to our choice of prior emissions but with the posterior emissions shifted towards the agricultural sector and less towards fossil emissions, consistent with our global posterior results. Our results suggest remote-sensing-based estimates of methane emissions can be substantially different (although within uncertainty) than bottom-up inventories, isotopic evidence, or estimates based on sparse in situ data, indicating a need for further studies reconciling these different approaches for quantifying the methane budget. Higher-resolution fluxes calculated from upcoming satellite or aircraft data such as the Tropospheric Monitoring Instrument (TROPOMI) and those in formulation such as the Copernicus CO2M, MethaneSat, or Carbon Mapper can be incorporated into our Bayesian estimation framework for the purpose of reducing uncertainty and improving the spatial resolution and sectoral attribution of subsequent methane emissions estimates.

The status of carbon neutrality of the world's top 5 CO2 emitters as seen by carbon satellites

China, the Unite States (US), the European Union (EU), India, and Russia are the world's top 5 fossil fuel and cement CO2 (FFC) emitting countries or regions (CRs). It is very important to understand their status of carbon neutrality, and to monitor their future changes of net carbon fluxes (NCFs). In this study, we implemented a well-established global carbon assimilation system (GCAS, Version 2) to infer global surface carbon fluxes from May 2009 to December 2019 using both GOSAT and OCO-2 XCO2 retrievals. The reductions of flux uncertainty and XCO2 bias, and the evaluation of posterior flux show that GCAS has comparable and good performance in the 5 CRs. The results suggest that Russia has achieved carbon neutrality, but the other 4 are still far from being carbon neutral, especially China. The mean annual NCFs in China, the US, the EU, India, and Russia are 2.33 ± 0.29, 0.82 ± 0.20, 0.42 ± 0.16, 0.50 ± 0.12, and -0.33 ± 0.23 PgC yr−1, respectively. From 2010 to 2019, the NCFs showed an increasing trend in the US and India, a slight downward trend after 2013 in China, and were stable in the EU. The changes of land sinks in China and the US might be the main reason for their trends. India's trend was mainly due to the increase of FFC emission. The relative contributions of NCFs to the global land net carbon emission of China and the EU have decreased, while those of the US and India have increased, implying the US and India must take more active measures to control carbon emissions or increase their sinks. This study indicates that satellite XCO2 could be successfully used to monitor the changes of regional NCFs, which is of great significance for major countries to achieve greenhouse gas control goals.

Variability of North Atlantic CO<sub>2</sub> fluxes for the 2000–2017 period estimated from atmospheric inverse analyses

Abstract. We present new estimates of the regional North Atlantic (15–80∘ N) CO2 flux for the 2000–2017 period using atmospheric CO2 measurements from the NOAA long-term surface site network in combination with an atmospheric carbon cycle data assimilation system (GEOS-Chem–LETKF, Local Ensemble Transform Kalman Filter). We assess the sensitivity of flux estimates to alternative ocean CO2 prior flux distributions and to the specification of uncertainties associated with ocean fluxes. We present a new scheme to characterize uncertainty in ocean prior fluxes, derived from a set of eight surface pCO2-based ocean flux products, and which reflects uncertainties associated with measurement density and pCO2-interpolation methods. This scheme provides improved model performance in comparison to fixed prior uncertainty schemes, based on metrics of model–observation differences at the network of surface sites. Long-term average posterior flux estimates for the 2000–2017 period from our GEOS-Chem–LETKF analyses are −0.255 ± 0.037 PgC yr−1 for the subtropical basin (15–50∘ N) and −0.203 ± 0.037 PgC yr−1 for the subpolar region (50–80∘ N, eastern boundary at 20∘ E). Our basin-scale estimates of interannual variability (IAV) are 0.036 ± 0.006 and 0.034 ± 0.009 PgC yr−1 for subtropical and subpolar regions, respectively. We find statistically significant trends in carbon uptake for the subtropical and subpolar North Atlantic of −0.064 ± 0.007 and −0.063 ± 0.008 PgC yr−1 decade−1; these trends are of comparable magnitude to estimates from surface ocean pCO2-based flux products, but they are larger, by a factor of 3–4, than trends estimated from global ocean biogeochemistry models.

Large and increasing methane emissions from eastern Amazonia derived from satellite data, 2010–2018

Abstract. We use a global inverse model, satellite data and flask measurements to estimate methane (CH4) emissions from South America, Brazil and the basin of the Amazon River for the period 2010–2018. We find that emissions from Brazil have risen during this period, most quickly in the eastern Amazon basin, and that this is concurrent with increasing surface temperatures in this region. Brazilian CH4 emissions rose from 49.8 ± 5.4 Tg yr−1 in 2010–2013 to 55.6 ± 5.2 Tg yr−1 in 2014–2017, with the wet season of December–March having the largest positive trend in emissions. Amazon basin emissions grew from 41.7 ± 5.3 to 49.3 ± 5.1 Tg yr−1 during the same period. We derive no significant trend in regional emissions from fossil fuels during this period. We find that our posterior distribution of emissions within South America is significantly and consistently changed from our prior estimates, with the strongest emission sources being in the far north of the continent and to the south and south-east of the Amazon basin, at the mouth of the Amazon River and nearby marsh, swamp and mangrove regions. We derive particularly large emissions during the wet season of 2013/14, when flooding was prevalent over larger regions than normal within the Amazon basin. We compare our posterior CH4 mole fractions, derived from posterior fluxes, to independent observations of CH4 mole fraction taken at five lower- to mid-tropospheric vertical profiling sites over the Amazon and find that our posterior fluxes outperform prior fluxes at all locations. In particular the large emissions from the eastern Amazon basin are shown to be in good agreement with independent observations made at Santarém, a location which has long displayed higher mole fractions of atmospheric CH4 in contrast with other basin locations. We show that a bottom-up wetland flux model can match neither the variation in annual fluxes nor the positive trend in emissions produced by the inversion. Our results show that the Amazon alone was responsible for 24 ± 18 % of the total global increase in CH4 flux during the study period, and it may contribute further in future due to its sensitivity to temperature changes.

Evaluation of CarbonTracker's Inverse Estimates of North American Net Ecosystem Exchange of CO2 From Different Observing Systems Using ACT‐America Airborne Observations

AbstractQuantification of regional terrestrial carbon dioxide (CO2) fluxes is critical to our understanding of the carbon cycle. We evaluate inverse estimates of net ecosystem exchange (NEE) of CO2 fluxes in temperate North America, and their sensitivity to the observational data used to drive the inversions. Specifically, we consider the state‐of‐the‐science CarbonTracker global inversion system, which assimilates (a) in situ measurements (IS), (b) the Orbiting Carbon Observatory‐2 (OCO‐2) v9 column CO2 (XCO2) retrievals over land (LNLG), (c) OCO‐2 v9 XCO2 retrievals ocean‐glint (OG), and (d) a combination of all these observational constraints (LNLGOGIS). We use independent CO2 observations from the Atmospheric Carbon and Transport (ACT)—America aircraft mission to evaluate the inversions. We diagnose errors in the flux estimates using the differences between modeled and observed biogenic CO2 mole fractions, influence functions from a Lagrangian transport model, Bayesian inference, and root‐mean‐square error (RMSE) and bias metrics. The IS fluxes have the smallest RMSE among the four products, followed by LNLG. Both IS and LNLG outperform the OG and LNLGOGIS inversions with regard to RMSE. Regional errors do not differ markedly across the four sets of posterior fluxes. The CarbonTracker inversions appear to overestimate the seasonal cycle of NEE in the Midwest and Western Canada, and overestimate dormant season NEE across the Central and Eastern US. The CarbonTracker inversions may overestimate annual NEE in the Central and Eastern US. The success of the LNLG inversion with respect to independent observations bodes well for satellite‐based inversions in regions with more limited in situ observing networks.

Improved Constraints on Northern Extratropical CO2 Fluxes Obtained by Combining Surface‐Based and Space‐Based Atmospheric CO2 Measurements

AbstractTop‐down estimates of CO2 fluxes are typically constrained by either surface‐based or space‐based CO2 observations. Both of these measurement types have spatial and temporal gaps in observational coverage that can lead to differences in inferred fluxes. Assimilating both surface‐based and space‐based measurements concurrently in a flux inversion framework improves observational coverage and reduces sampling related artifacts. This study examines the consistency of flux constraints provided by these different observations and the potential to combine them by performing a series of 6‐year (2010–2015) CO2 flux inversions. Flux inversions are performed assimilating surface‐based measurements from the in situ and flask network, measurements from the Total Carbon Column Observing Network (TCCON), and space‐based measurements from the Greenhouse Gases Observing Satellite (GOSAT), or all three data sets combined. Combining the data sets results in more precise flux estimates for subcontinental regions relative to any of the data sets alone. Combining the data sets also improves the accuracy of the posterior fluxes, based on reduced root‐mean‐square differences between posterior flux‐simulated CO2 and aircraft‐based CO2 over midlatitude regions (0.33–0.56 ppm) in comparison to GOSAT (0.37–0.61 ppm), TCCON (0.50–0.68 ppm), or in situ and flask measurements (0.46–0.56 ppm) alone. These results suggest that surface‐based and GOSAT measurements give complementary constraints on CO2 fluxes in the northern extratropics and can be combined in flux inversions to improve constraints on regional fluxes. This stands in contrast with many earlier attempts to combine these data sets and suggests that improvements in the NASA Atmospheric CO2 Observations from Space (ACOS) retrieval algorithm have significantly improved the consistency of space‐based and surface‐based flux constraints.

Representing model uncertainty for global atmospheric CO<sub>2</sub> flux inversions using ECMWF-IFS-46R1

Abstract. Atmospheric flux inversions use observations of atmospheric CO2 to provide anthropogenic and biogenic CO2 flux estimates at a range of spatio-temporal scales. Inversions require prior flux, a forward model and observation errors to estimate posterior fluxes and uncertainties. Here, we investigate the forward transport error and the associated biogenic feedback in an Earth system model (ESM) context. These errors can occur from uncertainty in the initial meteorology, the analysis fields used, or the advection schemes and physical parameterisation of the model. We also explore the spatio-temporal variability and flow-dependent error covariances. We then compare the error with the atmospheric response to uncertainty in the prior anthropogenic emissions. Although transport errors are variable, average total-column CO2 (XCO2) transport errors over anthropogenic emission hotspots (0.1–0.8 ppm) are comparable to, and often exceed, prior monthly anthropogenic flux uncertainties projected onto the same space (0.1–1.4 ppm). Average near-surface transport errors at three sites (Paris, Caltech and Tsukuba) range from 1.7 to 7.2 ppm. The global average XCO2 transport error standard deviation plateaus at ∼0.1 ppm after 2–3 d, after which atmospheric mixing significantly dampens the concentration gradients. Error correlations are found to be highly flow dependent, with XCO2 spatio-temporal correlation length scales ranging from 0 to 700 km and 0 to 260 min. Globally, the average model error caused by the biogenic response to atmospheric meteorological uncertainties is small (<0.01 ppm); however, this increases over high flux regions and is seasonally dependent (e.g. the Amazon; January and July: 0.24±0.18 ppm and 0.13±0.07 ppm). In general, flux hotspots are well-correlated with model transport errors. Our model error estimates, combined with the atmospheric response to anthropogenic flux uncertainty, are validated against three Total Carbon Observing Network (TCCON) XCO2 sites. Results indicate that our model and flux uncertainty account for 21 %–65 % of the total uncertainty. The remaining uncertainty originates from additional sources, such as observation, numerical and representation errors, as well as structural errors in the biogenic model. An underrepresentation of transport and flux uncertainties could also contribute to the remaining uncertainty. Our quantification of CO2 transport error can be used to help derive accurate posterior fluxes and error reductions in future inversion systems. The model uncertainty diagnosed here can be used with varying degrees of complexity and with different modelling techniques by the inversion community.

New constraints on biogenic emissions using satellite-based estimates of carbon monoxide fluxes

Abstract. Biogenic non-methane volatile organic compounds (NMVOCs) emitted from vegetation are a primary source for the chemical production of carbon monoxide (CO) in the atmosphere, and these biogenic emissions account for about 18 % of the global CO burden. Partitioning CO fluxes to different source types in top-down inversion methods is challenging; typically a simple scaling of the posterior flux to prior flux values for fossil fuel, biogenic and biomass burning sources is used. Here we show top-down estimates of biogenic CO fluxes using a Bayesian inference approach, which explicitly accounts for both posterior and a priori CO flux uncertainties. This approach re-partitions CO fluxes following inversion of Measurements Of Pollution In The Troposphere (MOPITT) CO observations with the GEOS-Chem model, a global chemical transport model driven by assimilated meteorology from the NASA Goddard Earth Observing System (GEOS). We compare these results to the prior information for CO used to represent biogenic NMVOCs from GEOS-Chem, which uses the Model of Emissions of Gases and Aerosols from Nature (MEGAN) for biogenic emissions. We evaluate the a posteriori biogenic CO fluxes against top-down estimates of isoprene fluxes using Ozone Monitoring Instrument (OMI) formaldehyde observations. We find similar seasonality and spatial consistency in the posterior CO and top-down isoprene estimates globally. For the African savanna region, both top-down CO and isoprene seasonality vary significantly from the MEGAN a priori inventory. This method for estimating biogenic sources of CO will provide an independent constraint on modeled biogenic emissions and has the potential for diagnosing decadal-scale changes in emissions due to land-use change and climate variability.

An atmospheric inversion over the city of Cape Town: sensitivity analyses

Abstract. An atmospheric inversion was performed for the city of Cape Town for the period of March 2012 to June 2013, making use of in situ measurements of CO2 concentrations at temporary measurement sites located to the north-east and south-west of Cape Town. This paper presents results of sensitivity analyses that tested assumptions regarding the prior information and the uncertainty covariance matrices associated with the prior fluxes and with the observations. Alternative prior products were considered in the form of a carbon assessment analysis to provide biogenic fluxes and the ODIAC (Open-source Data Inventory for Anthropogenic CO2 product) fossil fuel product. These were used in place of the reference inversion's biogenic fluxes from CABLE (Community Atmosphere Biosphere Land Exchange model) and fossil fuel emissions from a bespoke inventory analysis carried out specifically for the Cape Town inversion. Our results confirmed that the inversion solution was strongly dependent on the prior information, but by using independent alternative prior products to run multiple inversions, we were able to infer limits for the true domain flux. Where the reference inversion had aggregated prior flux estimates that were made more positive by the inversion – suggesting that CABLE was overestimating the amount of CO2 biogenic uptake – the carbon assessment prior fluxes were made more negative by the inversion. As the posterior estimates tended towards the same point, we could infer that the best estimate was located somewhere between these two posterior fluxes. The inversion was shown to be sensitive to the spatial error correlation length in the biogenic fluxes – even a short correlation length – influencing the spatial distribution of the posterior fluxes, the size of the aggregated flux across the domain, and the uncertainty reduction achieved by the inversion. Taking advantage of expected spatial correlations in the fluxes is key to maximizing the use of a limited observation network. Changes to the temporal correlations in the observation errors had a very minor effect on the inversion. The control vector in the original version consisted of separate daytime and night-time weekly fluxes for fossil fuel and biogenic fluxes over a 4-week inversion period. When we considered solving for mean weekly fluxes over each 4-week period – i.e. assuming the flux remained constant over the month – larger changes to the prior fossil fuel and biogenic fluxes were possible, as well as further changes to the spatial distribution of the fluxes compared with the reference. The uncertainty reduction achieved in the estimation of the overall flux increased from 25.6 % for the reference inversion to 47.2 % for the mean weekly flux inversion. This demonstrates that if flux components that change slowly can be solved for separately in the inversion, where these fluxes are assumed to be constant over long periods of time, the posterior estimates of these fluxes substantially benefit from the additional observational constraint. In summary, estimates of Cape Town fluxes can be improved by using better and multiple prior information sources, and particularly on biogenic fluxes. Fossil fuel and biogenic fluxes should be broken down into components, building in knowledge of spatial and temporal consistency in these components into the control vector and uncertainties specified for the sources for the inversion. This would allow the limited observations to provide maximum constraint on the flux estimates.

Inversion Estimates of Lognormally Distributed Methane Emission Rates From the Haynesville‐Bossier Oil and Gas Production Region Using Airborne Measurements

AbstractQuantifying methane (CH4) emissions from the oil and natural gas (O/NG) production sector is an important regulatory challenge in the United States. In this study, we conduct a set of inversion calculations using different methods to quantify lognormal distributed CH4 surface fluxes in the Haynesville‐Bossier O/NG production basin in Texas and Louisiana, combining three statistical cost functions, four meteorological configurations, and two days of aircraft measurements from a 2013 field campaign. We aggregate our posterior flux estimates to derive our best estimate of the basin‐wide CH4 emissions, 76 metric tons/hr, with a 95% highest density interval of 51–104 metric tons/hr, in agreement with previous estimates using mass balance and eddy covariance approaches with the same aircraft measurements. Our inversion estimate of basin‐wide CH4 emissions is 133% (89%–182%, 95% highest density interval) of a gridded Environmental Protection Agency's inventory for 2012, and the largest discrepancies between our study and this inventory are located in the northeastern quadrant of the basin containing active unconventional O/NG wells. Our inversion approach provides a new spatiotemporal characterization of CH4 emissions in this O/NG production region and shows the usefulness of inverse modeling for improving O/NG CH4 emission estimates.

Attribution of recent increases in atmospheric methane through 3-D inverse modelling

Abstract. The atmospheric methane (CH4) growth rate has varied considerably in recent decades. Unexplained renewed growth after 2006 followed 7 years of stagnation and coincided with an isotopic trend toward CH4 more depleted in 13C, suggesting changes in sources and/or sinks. Using surface observations of both CH4 and the relative change of isotopologue ratio (δ13CH4) to constrain a global 3-D chemical transport model (CTM), we have performed a synthesis inversion for source and sink attribution. Our method extends on previous studies by providing monthly and regional attribution of emissions from six different sectors and changes in atmospheric sinks for the extended 2003–2015 period. Regional evaluation of the model CH4 tracer with independent column observations from the Greenhouse Gases Observing Satellite (GOSAT) shows improved performance when using posterior fluxes (R=0.94–0.96, RMSE =8.3–16.5 ppb), relative to prior fluxes (R=0.60–0.92, RMSE =48.6–64.6 ppb). Further independent validation with data from the Total Carbon Column Observing Network (TCCON) shows a similar improvement in the posterior fluxes (R=0.87, RMSE =18.8 ppb) compared to the prior fluxes (R=0.69, RMSE =55.9 ppb). Based on these improved posterior fluxes, the inversion results suggest the most likely cause of the renewed methane growth is a post-2007 1.8±0.4 % decrease in mean OH, a 12.9±2.7 % increase in energy sector emissions, mainly from Africa–Middle East and southern Asia–Oceania, and a 2.6±1.8 % increase in wetland emissions, mainly from northern Eurasia. The posterior wetland flux increases are in general agreement with bottom-up estimates, but the energy sector growth is greater than estimated by bottom-up methods. The model results are consistent across a range of sensitivity analyses. When forced to assume a constant (annually repeating) OH distribution, the inversion requires a greater increase in energy sector (13.6±2.7 %) and wetland (3.6±1.8 %) emissions and an 11.5±3.8 % decrease in biomass burning emissions. Assuming no prior trend in sources and sinks slightly reduces the posterior growth rate in energy sector and wetland emissions and further increases the magnitude of the negative OH trend. We find that possible tropospheric Cl variations do not influence δ13CH4 and CH4 trends, although we suggest further work on Cl variability is required to fully diagnose this contribution. While the study provides quantitative insight into possible emissions variations which may explain the observed trends, uncertainty in prior source and sink estimates and a paucity of δ13CH4 observations limit the robustness of the posterior estimates.

A comparison of posterior atmospheric CO<sub>2</sub> adjustments obtained from in situ and GOSAT constrained flux inversions

Abstract. Posterior fluxes obtained from inverse modelling are difficult to verify because there is no dense network of flux measurements available to evaluate estimates against. Here we present a new diagnostic to evaluate structures in posterior fluxes. First, we simulate the change in atmospheric CO2 fields between posterior and prior fluxes, referred to as the posterior atmospheric adjustments due to updated fluxes (PAAFs). Second, we calculate the uncertainty in atmospheric CO2 fields due solely to uncertainty in the meteorological fields, referred to as the posterior atmospheric adjustments due to imperfect meteorology (PAAMs). We argue that PAAF can only be considered robust if it exceeds PAAM, that is, the changes in atmospheric CO2 between the posterior and prior fluxes should at least exceed atmospheric CO2 changes arising from imperfect meteorology. This diagnostic is applied to two CO2 flux inversions: one which assimilates observations from the in situ CO2 network and the other which assimilates observations from the Greenhouse Gases Observing SATellite (GOSAT). On the global scale, PAAF in the troposphere reflects northern extratropical fluxes, whereas stratospheric adjustments primarily reflect tropical fluxes. In general, larger spatiotemporal variations in PAAF are obtained for the GOSAT inversion than for the in situ inversion. Zonal standard deviations of the PAAF exceed the PAAM through most of the year when GOSAT observations are used, but the minimum value is exceeded only in boreal summer when in situ observations are used. Zonal spatial structures in GOSAT-based PAAF exceed PAAM throughout the year in the tropics and through most of the year in the northern extratropics, suggesting GOSAT flux inversions can constrain zonal asymmetries in fluxes. However, we cannot discount the possibility that these structures are influenced by biases in GOSAT retrievals. Verification of such spatial structures will require a dense network of independent observations. Because PAAF depends on the choice of prior fluxes, the comparison with PAAM is system dependent and thus can be used to monitor a given assimilation system's behaviour.

Atmospheric CO<sub>2</sub> inversions on the mesoscale using data-driven prior uncertainties: quantification of the European terrestrial CO<sub>2</sub> fluxes

Abstract. Optimized biogenic carbon fluxes for Europe were estimated from high-resolution regional-scale inversions, utilizing atmospheric CO2 measurements at 16 stations for the year 2007. Additional sensitivity tests with different data-driven error structures were performed. As the atmospheric network is rather sparse and consequently contains large spatial gaps, we use a priori biospheric fluxes to further constrain the inversions. The biospheric fluxes were simulated by the Vegetation Photosynthesis and Respiration Model (VPRM) at a resolution of 0.1° and optimized against eddy covariance data. Overall we estimate an a priori uncertainty of 0.54 GtC yr−1 related to the poor spatial representation between the biospheric model and the ecosystem sites. The sink estimated from the atmospheric inversions for the area of Europe (as represented in the model domain) ranges between 0.23 and 0.38 GtC yr−1 (0.39 and 0.71 GtC yr−1 up-scaled to geographical Europe). This is within the range of posterior flux uncertainty estimates of previous studies using ground-based observations.

Constraining a terrestrial biosphere model with remotely sensed atmospheric carbon dioxide

We present two novel earth observation products derived from the BESD and EMMA XCO2 products which were respectively retrieved from SCIAMACHY and GOSAT observations within the GreenHouse Gas project of ESA's Climate Change Initiative (GHG-CCI). These products are inferred by a Carbon Cycle Data Assimilation System (CCDAS) and consist of net and gross biosphere-atmosphere fluxes of carbon dioxide on a global 0.5° grid. As a further dataset provided by the CCI, the burnt area product developed by its Fire忌i project was used in the CCDAS to prescribe the emission component from biomass burning. The new flux products are provided with per-pixel uncertainty ranges. Fluxes with uncertainty ranges can also be provided aggregated in space and time, e.g. over given regions or as annual means. For both, posterior flux fields inferred from BESD and EMMA products, transport model simulations show reasonable agreement with the atmospheric carbon dioxide concentration observed at flask sampling stations. This means that the information provided by the terrestrial and transport models, the respective GHG ECV product, the burnt area ECV product, a product of the Fraction of Absorbed Photosynthetically Active Radiation used to drive the model, and the atmospheric flask samples is largely consistent.The most prominent feature in the posterior net flux is the tropical source of CO2 inferred from both products. But for the EMMA product this release, especially over South America, is with 300gC/m2/year much more pronounced than for BESD. This confirms findings by a recent intercomparison of transport inversions using GOSAT data by Houweling et al. (2015). The reason for the larger net flux is increased heterotrophic respiration. For both products the posterior 2010 sink over Europe (without Russia) is in the range of a recent compilation of European flux estimates by Reuter et al. (2016b). The posterior 2010 uptake of Australia (including Oceania) inferred from the EMMA product is 1.3 ± 0.2PgC/year and appears to confirm the high sink also derived from GOSAT by Detmers et al. (2015) over a slightly different period and area. While for some regions (USA, Canada, Europe, Russia, Asia) the one standard deviation uncertainty ranges derived from BESD and EMMA do overlap, for some other regions (Brazil, Africa, Australia) this is not the case. It is not clear yet whether this is due to the uncertainty specifications in the respective products or the handling of uncertainty in the assimilation chain. Assumptions on correlation of observational uncertainty in space and time have a considerable impact on the inferred flux fields (≈ 60gC/m2/year). The effect of adding an uncertainty that approximates the error in the retrieval system is of similar size.

A global wetland methane emissions and uncertainty dataset for atmospheric chemical transport models (WetCHARTs version 1.0)

Abstract. Wetland emissions remain one of the principal sources of uncertainty in the global atmospheric methane (CH4) budget, largely due to poorly constrained process controls on CH4 production in waterlogged soils. Process-based estimates of global wetland CH4 emissions and their associated uncertainties can provide crucial prior information for model-based top-down CH4 emission estimates. Here we construct a global wetland CH4 emission model ensemble for use in atmospheric chemical transport models (WetCHARTs version 1.0). Our 0.5° × 0.5° resolution model ensemble is based on satellite-derived surface water extent and precipitation reanalyses, nine heterotrophic respiration simulations (eight carbon cycle models and a data-constrained terrestrial carbon cycle analysis) and three temperature dependence parameterizations for the period 2009–2010; an extended ensemble subset based solely on precipitation and the data-constrained terrestrial carbon cycle analysis is derived for the period 2001–2015. We incorporate the mean of the full and extended model ensembles into GEOS-Chem and compare the model against surface measurements of atmospheric CH4; the model performance (site-level and zonal mean anomaly residuals) compares favourably against published wetland CH4 emissions scenarios. We find that uncertainties in carbon decomposition rates and the wetland extent together account for more than 80 % of the dominant uncertainty in the timing, magnitude and seasonal variability in wetland CH4 emissions, although uncertainty in the temperature CH4 : C dependence is a significant contributor to seasonal variations in mid-latitude wetland CH4 emissions. The combination of satellite, carbon cycle models and temperature dependence parameterizations provides a physically informed structural a priori uncertainty that is critical for top-down estimates of wetland CH4 fluxes. Specifically, our ensemble can provide enhanced information on the prior CH4 emission uncertainty and the error covariance structure, as well as a means for using posterior flux estimates and their uncertainties to quantitatively constrain the biogeochemical process controls of global wetland CH4 emissions.

The constraint of CO<sub>2</sub> measurements made onboard passenger aircraft on surface–atmosphere fluxes: the impact of transport model errors in vertical mixing

Abstract. Inaccurate representation of atmospheric processes by transport models is a dominant source of uncertainty in inverse analyses and can lead to large discrepancies in the retrieved flux estimates. We investigate the impact of uncertainties in vertical transport as simulated by atmospheric transport models on fluxes retrieved using vertical profiles from aircraft as an observational constraint. Our numerical experiments are based on synthetic data with realistic spatial and temporal sampling of aircraft measurements. The impact of such uncertainties on the flux retrieved using the ground-based network and those retrieved using the aircraft profiles are compared. We find that the posterior flux retrieved using aircraft profiles is less susceptible to errors in boundary layer height, compared to the ground-based network. This finding highlights a benefit of utilizing atmospheric observations made onboard aircraft over surface measurements for flux estimation using inverse methods. We further use synthetic vertical profiles of CO2 in an inversion to estimate the potential of these measurements, which will be made available through the IAGOS (In-service Aircraft for a Global Observing System) project in the future, in constraining the regional carbon budget. Our results show that the regions of tropical Africa and temperate Eurasia, that are under-constrained by the existing surface-based network, will benefit the most from these measurements, with a reduction of posterior flux uncertainty of about 7 to 10 %.