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Optimal estimation retrievals of trace gas total columns require prior vertical profiles of the gases retrieved to drive the forward model and ensure the retrieval problem is mathematically well posed. For well-mixed gases, it is possible to derive accurate prior profiles using an algorithm that accounts for general patterns of atmospheric transport coupled with measured time series of the gases in questions. Here we describe the algorithm used to generate the prior profiles for GGG2020, a new version of the GGG retrieval that is used to analyze spectra from solar-viewing Fourier transform spectrometers, including the Total Carbon Column Observing Network (TCCON). A particular focus of this work is improving the accuracy of CO2, CH4, N2O, HF, and CO across the tropopause and into the lower stratosphere. We show that the revised priors agree well with independent in situ and space-based measurements and discuss the impact on the total column retrievals.

Approximately half of the carbon dioxide (CO 2) released annually by the combustion of fossil fuels stays in the atmosphere (Friedlingstein et al., 2022; Keeling et al., 1976; Schimel et al., 2001). The remaining CO 2 is taken up by the terrestrial biosphere and ocean in roughly equal proportions (Keeling & Manning, 2014; Khatiwala et al., 2009; Sabine et al., 2004). The efficiency of the ocean and land sinks varies with both climate and atmospheric CO 2 , representing an important feedback in the climate system (e.g., Ballantyne et al., 2012

This article provides an overview of the NASA Atmospheric Tomography (ATom) mission and a summary of selected scientific findings to date. ATom was an airborne measurements and modeling campaign aimed at characterizing the composition and chemistry of the troposphere over the most remote regions of the Pacific, Southern, Atlantic, and Arctic Oceans, and examining the impact of anthropogenic and natural emissions on a global scale. These remote regions dominate global chemical reactivity and are exceptionally important for global air quality and climate. ATom data provide the in situ measurements needed to understand the range of chemical species and their reactions, and to test satellite remote sensing observations and global models over large regions of the remote atmosphere. Lack of data in these regions, particularly over the oceans, has limited our understanding of how atmospheric composition is changing in response to shifting anthropogenic emissions and physical climate change. ATom was designed as a global-scale tomographic sampling mission with extensive geographic and seasonal coverage, tropospheric vertical profiling, and detailed speciation of reactive compounds and pollution tracers. ATom flew the NASA DC-8 research aircraft over four seasons to collect a comprehensive suite of measurements of gases, aerosols, and radical species from the remote troposphere and lower stratosphere on four global circuits from 2016 to 2018. Flights maintained near-continuous vertical profiling of 0.15–13-km altitudes on long meridional transects of the Pacific and Atlantic Ocean basins. Analysis and modeling of ATom data have led to the significant early findings highlighted here.

Wintertime episodes of high aerosol concentrations occur frequently in urban and agricultural basins and valleys worldwide. These episodes often arise following development of persistent cold-air pools (PCAPs) that limit mixing and modify chemistry. While field campaigns targeting either basin meteorology or wintertime pollution chemistry have been conducted, coupling between interconnected chemical and meteorological processes remains an insufficiently studied research area. Gaps in understanding the coupled chemical–meteorological interactions that drive high-pollution events make identification of the most effective air-basin specific emission control strategies challenging. To address this, a September 2019 workshop occurred with the goal of planning a future research campaign to investigate air quality in western U.S. basins. Approximately 120 people participated, representing 50 institutions and five countries. Workshop participants outlined the rationale and design for a comprehensive wintertime study that would couple atmospheric chemistry and boundary layer and complex-terrain meteorology within western U.S. basins. Participants concluded the study should focus on two regions with contrasting aerosol chemistry: three populated valleys within Utah (Salt Lake, Utah, and Cache Valleys) and the San Joaquin Valley in California. This paper describes the scientific rationale for a campaign that will acquire chemical and meteorological datasets using airborne platforms with extensive range, coupled to surface-based measurements focusing on sampling within the near-surface boundary layer, and transport and mixing processes within this layer, with high vertical resolution at a number of representative sites. No prior wintertime basin-focused campaign has provided the breadth of observations necessary to characterize the meteorological–chemical linkages outlined here, nor to validate complex processes within coupled atmosphere–chemistry models.

Accurate simulation of atmospheric circulation, particularly in the lower stratosphere, is challenging due to unresolved wave-mean flow interactions and limited high-resolution observations for validation. Gravity-induced pressure gradients lead to a small but measurable separation of heavy and light gases by molecular diffusion in the stratosphere. Because the relative abundance of Ar to N2 is exclusively controlled by physical transport, the argon-to-nitrogen ratio (Ar/N2) provides an additional constraint on circulation and the age of air (AoA), i.e. the time elapsed since entry of an air parcel into the stratosphere. Here we use airborne measurements of N2O and Ar/N2 from nine campaigns with global coverage spanning 2008–2018 to calculate AoA and to quantify gravitational separation in the lowermost stratosphere. To this end, we develop a new N2O-AoA relationship using a Markov Chain Monte Carlo algorithm. We observe that gravitational separation increases systematically with increasing AoA for samples with AoA between 0 to 3 years. These observations are compared to a simulation of the TOMCAT/SLIMCAT 3-D chemical transport model, which has been updated to include gravitational fractionation of gases. We demonstrate that although AoA at old ages is slightly underestimated in the model, the relationship between Ar/N2 and AoA is robust and agrees with the observations. This highlights the potential of Ar/N2 to become a new AoA tracer that is subject only to physical transport phenomena and can supplement the suite of available AoA indicators.

20 pags., 11 figs. 1 tab. -- Open Access funded by Creative Commons Atribution Licence 4.0, Fluxes of halogenated volatile organic compounds (VOCs) over the Southern Ocean remain poorly understood, and few atmospheric measurements exist to constrain modeled emissions of these compounds. We present observations of CHBr, CHBr, CHI, CHClBr, CHBrCl, and CHBr during the O2=N Ratio and CO Airborne Southern Ocean (ORCAS) study and the second Atmospheric Tomography mission (ATom-2) in January and February of 2016 and 2017. Good model-measurement correlations were obtained between these observations and simulations from the Community Earth System Model (CESM) atmospheric component with chemistry (CAM-Chem) for CHBr, CHBr, CHI, and CHClBr but all showed significant differences in model: measurement ratios. The model: measurement comparison for CHBr was satisfactory and for CHBrCl the low levels present precluded us from making a complete assessment. Thereafter, we demonstrate two novel approaches to estimate halogenated VOC fluxes; the first approach takes advantage of the robust relationships that were found between airborne observations of O and CHBr, CHBr, and CHClBr. We use these linear regressions with O and modeled O distributions to infer a biological flux of halogenated VOCs. The second approach uses the Stochastic Time-Inverted Lagrangian Transport (STILT) particle dispersion model to explore the relationships between observed mixing ratios and the product of the upstream surface influence of sea ice, chl a, absorption due to detritus, and downward shortwave radiation at the surface, which in turn relate to various regional hypothesized sources of halogenated VOCs such as marine phytoplankton, phytoplankton in seaice brines, and decomposing organic matter in surface seawater. These relationships can help evaluate the likelihood of particular halogenated VOC sources and in the case of statistically significant correlations, such as was found for CHI, may be used to derive an estimated flux field. Our results are consistent with a biogenic regional source of CHBr and both nonbiological and biological sources of CHI over these regions., We would like to thank the ORCAS and ATom-2 science teams as well as the NCAR Research Aviation Facility and NASA DC-8 pilots, technicians, and mechanics for their support during the field campaigns. This work was made possible by grants from NSF Polar Programs (1501993, 1501997, 1501292, 1502301, 1543457), NSF Atmospheric Chemistry grants 1535364, 1623745, and 1623748, and NASA funding of the EVS2 Atmospheric Tomography (ATom) project, as well as the support of the NCAR Advanced Study Program (ASP) Postdoctoral Fellowship Program and computing support from Yellowstone, provided by NCAR’s Computational and Information Systems Laboratory. The National Center for Atmospheric Research is sponsored by the National Science Foundation. Financial support.

The Southern Ocean plays an important role in determining atmospheric carbon dioxide (CO2), yet estimates of air-sea CO2 flux for the region diverge widely. In this study, we constrained Southern Ocean air-sea CO2 exchange by relating fluxes to horizontal and vertical CO2 gradients in atmospheric transport models and applying atmospheric observations of these gradients to estimate fluxes. Aircraft-based measurements of the vertical atmospheric CO2 gradient provide robust flux constraints. We found an annual mean flux of –0.53 ± 0.23 petagrams of carbon per year (net uptake) south of 45°S during the period 2009–2018. This is consistent with the mean of atmospheric inversion estimates and surface-ocean partial pressure of CO2 (PCO2)–based products, but our data indicate stronger annual mean uptake than suggested by recent interpretations of profiling float observations.

Cloud phase and relative humidity (RH) distributions at −67° to 0°C over the Southern Ocean during austral summer are compared between in situ airborne observations and global climate simulations. A scale-aware comparison is conducted using horizontally averaged observations from 0.1 to 50 km. Cloud phase frequencies, RH distributions, and liquid mass fraction are found to be less affected by horizontal resolutions than liquid and ice water content (LWC and IWC, respectively), liquid and ice number concentrations (Ncliq and Ncice, respectively), and ice supersaturation (ISS) frequency. At −10° to 0°C, observations show 27%–34% and 17%–37% of liquid and mixed phases, while simulations show 60%–70% and 3%–4%, respectively. Simulations overestimate (underestimate) LWC and Ncliq in liquid (mixed) phase, overestimate Ncice in mixed phase, underestimate IWC in ice and mixed phases, and underestimate (overestimate) liquid mass fraction below (above) −5°C, indicating that observational constraints are needed for different cloud phases. RH frequently occurs at liquid saturation in liquid and mixed phases for all datasets, yet the observed RH in ice phase can deviate from liquid saturation by up to 20%–40% at −20° to 0°C, indicating that the model assumption of liquid saturation for coexisting ice and liquid is inaccurate for low liquid mass fractions (

We have compared a suite of recent global CO2 atmospheric inversion results to independent airborne observations and to each other, to assess their dependence on differences in northern extratropical (NET) vertical transport and to identify some of the drivers of model spread. We evaluate posterior CO2 concentration profiles against observations from the High-Performance Instrumented Airborne Platform for Environmental Research (HIAPER) Pole-to-Pole Observations (HIPPO) aircraft campaigns over the mid-Pacific in 2009–2011. Although the models differ in inverse approaches, assimilated observations, prior fluxes, and transport models, their broad latitudinal separation of land fluxes has converged significantly since the Atmospheric Carbon Cycle Inversion Intercomparison (TransCom 3) and the REgional Carbon Cycle Assessment and Processes (RECCAP) projects, with model spread reduced by 80 % since TransCom 3 and 70 % since RECCAP. Most modeled CO2 fields agree reasonably well with the HIPPO observations, specifically for the annual mean vertical gradients in the Northern Hemisphere. Northern Hemisphere vertical mixing no longer appears to be a dominant driver of northern versus tropical (T) annual flux differences. Our newer suite of models still gives northern extratropical land uptake that is modest relative to previous estimates (Gurney et al., 2002; Peylin et al., 2013) and near-neutral tropical land uptake for 2009–2011. Given estimates of emissions from deforestation, this implies a continued uptake in intact tropical forests that is strong relative to historical estimates (Gurney et al., 2002; Peylin et al., 2013). The results from these models for other time periods (2004–2014, 2001–2004, 1992–1996) and re-evaluation of the TransCom 3 Level 2 and RECCAP results confirm that tropical land carbon fluxes including deforestation have been near neutral for several decades. However, models still have large disagreements on ocean–land partitioning. The fossil fuel (FF) and the atmospheric growth rate terms have been thought to be the best-known terms in the global carbon budget, but we show that they currently limit our ability to assess regional-scale terrestrial fluxes and ocean–land partitioning from the model ensemble.

A new airborne system, the Whole Air Sampling Pilotless Platform (WASPP), is described for the collection of whole air samples and in situ meteorological measurements onboard a commercial hexacopter. Rapid sample collection enables the collection ≤15 air samples per flight in positively pressurized miniature canisters, subsequently analyzed on a mated analytical system for up to 80 nonmethane volatile organic compounds (VOCs). The WASPP is well suited to investigate VOC gradients in urban environments impacted by traffic, industry, and oil and natural gas (O&NG) development, but has the sensitivity to characterize continental background conditions, as shown here using a subset of >40 species. We document empirical tests to minimize the influence of rotor wash and other sampling artifacts and report favorable results of laboratory-based calibrations of the WASPP's meteorological sensors and field-based comparisons of WASPP's VOC measurements and horizontal wind velocity measurements. Airborne WASPP measurements can complement and enhance ground-based VOC monitoring efforts by providing substantial meteorological and VOC measurement capability across vertical and horizontal spatial scales. These measurements reveal strong vertical gradients in VOC mixing ratios, depending on local meteorology and sources. WASPP has wide applicability for pollution source identification and quantification of hazardous air pollutants and precursors of criteria pollutants, including monitoring O&NG emissions or industry fenceline monitoring.

We introduce a transformed isentropic coordinate Mθe, defined as the dry air mass under a given equivalent potential temperature surface (θe) within a hemisphere. Like θe, the coordinate Mθe follows the synoptic distortions of the atmosphere but, unlike θe, has a nearly fixed relationship with latitude and altitude over the seasonal cycle. Calculation of Mθe is straightforward from meteorological fields. Using observations from the recent HIAPER Pole-to-Pole Observations (HIPPO) and Atmospheric Tomography Mission (ATom) airborne campaigns, we map the CO2 seasonal cycle as a function of pressure and Mθe, where Mθe is thereby effectively used as an alternative to latitude. We show that the CO2 seasonal cycles are more constant as a function of pressure using Mθe as the horizontal coordinate compared to latitude. Furthermore, short-term variability in CO2 relative to the mean seasonal cycle is also smaller when the data are organized by Mθe and pressure than when organized by latitude and pressure. We also present a method using Mθe to compute mass-weighted averages of CO2 on a hemispheric scale. Using this method with the same airborne data and applying corrections for limited coverage, we resolve the average CO2 seasonal cycle in the Northern Hemisphere (mass-weighted tropospheric climatological average for 2009–2018), yielding an amplitude of 7.8 ± 0.14 ppm and a downward zero-crossing on Julian day 173 ± 6.1 (i.e., late June). Mθe may be similarly useful for mapping the distribution and computing inventories of any long-lived chemical tracer.

We introduce a transformed isentropic coordinate Mθe, defined as the dry air mass under a given equivalent potential temperature surface (θe) within a hemisphere. Like θe, the coordinate Mθe follows the synoptic distortions of the atmosphere, but unlike θe, has a nearly fixed relationship with latitude and altitude over the seasonal cycle. Calculation of Mθe is straightforward from meteorological fields. Using observations from the recent HIPPO and Atom airborne campaigns, we map the CO2 seasonal cycle as a function of pressure and Mθe, where Mθe is thereby effectively used as an alternative to latitude. We show that the CO2 cycles are more constant as a function of pressure using Mθe as the horizontal coordinate compared to latitude. Furthermore, short-term variability of CO2 relative to the mean seasonal cycle is also smaller when the data are organized by Mθe and pressure than when organized by latitude and pressure. We also present a method using Mθe to compute mass-weighted averages of CO2 on a hemispheric scale. Using this method with the same airborne data and applying corrections for limited coverage, we resolve the average CO2 seasonal cycle in the Northern Hemisphere (mass weighted tropospheric climatological average for 2009–2018), yielding an amplitude of 7.8 ± 0.14 ppm and a downward zero-crossing at Julian day 173 ± 6.1 (i.e., late June). Mθe may be similarly useful for mapping the distribution and computing inventories of any long-lived chemical tracer.

We have compared a suite of recent global CO2 atmospheric inversion results to independent airborne observations and to each other, to assess their dependence on differences in northern extratropical (NET) vertical transport and to identify some of the drivers of model spread. We evaluate posterior CO2 concentration profiles against observations from the High-Performance Instrumented Airborne Platform for Environmental Research (HIAPER) Pole-to-Pole Observations (HIPPO) aircraft campaigns over the mid-Pacific in 2009–2011. Although the models differ in inverse approaches, assimilated observations, prior fluxes, and transport models, their broad latitudinal separation of land fluxes has converged significantly since the Atmospheric Carbon Cycle Inversion Intercomparison (TransCom 3) and the REgional Carbon Cycle Assessment and Processes (RECCAP) projects, with model spread reduced by 80% since TransCom 3 and 70% since RECCAP. Most modeled CO2 fields agree reasonably well with the HIPPO observations, specifically for the annual mean vertical gradients in the Northern Hemisphere. Northern Hemisphere vertical mixing no longer appears to be a dominant driver of northern versus tropical (T) annual flux differences. Our newer suite of models still gives northern extratropical land uptake that is modest relative to previous estimates (Gurney et al., 2002; Peylin et al., 2013) and near-neutral tropical land uptake for 2009–2011. Given estimates of emissions from deforestation, this implies a continued uptake in intact tropical forests that is strong relative to historical estimates (Gurney et al., 2002; Peylin et al., 2013). The results from these models for other time periods (2004–2014, 2001–2004, 1992–1996) and reevaluation of the TransCom 3 Level 2 and RECCAP results confirm that tropical land carbon fluxes including deforestation have been near neutral for several decades. However, models still have large disagreements on ocean–land partitioning. The fossil fuel (FF) and the atmospheric growth rate terms have been thought to be the best-known terms in the global carbon budget, but we show that they currently limit our ability to assess regional-scale terrestrial fluxes and ocean–land partitioning from the model ensemble.

The Southern Ocean is highly under-sampled for the purpose of assessing total carbon uptake and its variability. Since this region dominates the mean global ocean sink for anthropogenic carbon, understanding temporal change is critical. Underway measurements of pCO2 collected as part of the Drake Passage Time-series (DPT) program that began in 2002 inform our understanding of seasonally changing air–sea gradients in pCO2, and by inference the carbon flux in this region. Here, we utilize available pCO2 observations to evaluate how the seasonal cycle, interannual variability, and long-term trends in surface ocean pCO2 in the Drake Passage region compare to that of the broader subpolar Southern Ocean. Our results indicate that the Drake Passage is representative of the broader region in both seasonality and long-term pCO2 trends, as evident through the agreement of timing and amplitude of seasonal cycles as well as trend magnitudes both seasonally and annually. The high temporal density of sampling by the DPT is critical to constraining estimates of the seasonal cycle of surface pCO2 in this region, as winter data remain sparse in areas outside of the Drake Passage. An increase in winter data would aid in reduction of uncertainty levels. On average over the period 2002–2016, data show that carbon uptake has strengthened with annual surface ocean pCO2 trends in the Drake Passage and the broader subpolar Southern Ocean less than the global atmospheric trend. Analysis of spatial correlation shows Drake Passage pCO2 to be representative of pCO2 and its variability up to several hundred kilometers away from the region. We also compare DPT data from 2016 and 2017 to contemporaneous pCO2 estimates from autonomous biogeochemical floats deployed as part of the Southern Ocean Carbon and Climate Observations and Modeling project (SOCCOM) so as to highlight the opportunity for evaluating data collected on autonomous observational platforms. Though SOCCOM floats sparsely sample the Drake Passage region for 2016–2017 compared to the Drake Passage Time-series, their pCO2 estimates fall within the range of underway observations given the uncertainty on the estimates. Going forward, continuation of the Drake Passage Time-series will reduce uncertainties in Southern Ocean carbon uptake seasonality, variability, and trends, and provide an invaluable independent dataset for post-deployment assessment of sensors on autonomous floats. Together, these datasets will vastly increase our ability to monitor change in the ocean carbon sink.

Numerous mountain valleys experience wintertime particulate pollution events, when persistent cold air pools (PCAPs) develop and inhibit atmospheric mixing, leading to the accumulation of pollutants. Here we examine the relationships between trace gases and criteria pollutants during winter in Utah's Salt Lake Valley, in an effort to better understand the roles of transport versus chemical processes during differing meteorological conditions as well as insights into how targeted reductions in greenhouse gases will impact local air quality in varying meteorological conditions. CO2 is a chemically inert gas that is coemitted during fossil fuel combustion with pollutants. Many of these coemitted pollutants are precursors that react chemically to form secondary particulate matter. Thus, CO2 can serve as a stable tracer and potentially help distinguish transport versus chemical influences on pollutants. During the winter of 2015–2016, we isolated enhancements in CO2 over baseline levels due to urban emissions (“CO2ex”). CO2ex was paired with similar excesses in other pollutant concentrations. These relationships were examined during different wintertime conditions and stages of pollution episodes: (a) Non-PCAP, (b) beginning, and (c) latter stages of an episode. We found that CO2ex is a good indicator of the presence of gaseous criteria pollutants and a reasonable indicator of PM2.5. Additionally, the relationships between CO2ex and criteria pollutants differ during different phases of PCAP events which provide insight into meteorological and transport processes. Lastly, we found a slight overestimation of CO:CO2 emission ratios and a considerable overestimation of NOx:CO2 by existing inventories for the Salt Lake Valley.

Cities are concentrated areas of CO2 emissions and have become the foci of policies for mitigation actions. However, atmospheric measurement networks suitable for evaluating urban emissions over time are scarce. Here we present a unique long-term (decadal) record of CO2 mole fractions from five sites across Utah's metropolitan Salt Lake Valley. We examine "excess" CO2 above background conditions resulting from local emissions and meteorological conditions. We ascribe CO2 trends to changes in emissions, since we did not find long-term trends in atmospheric mixing proxies. Three contrasting CO2 trends emerged across urban types: negative trends at a residential-industrial site, positive trends at a site surrounded by rapid suburban growth, and relatively constant CO2 over time at multiple sites in the established, residential, and commercial urban core. Analysis of population within the atmospheric footprints of the different sites reveals approximately equal increases in population influencing the observed CO2, implying a nonlinear relationship with CO2 emissions: Population growth in rural areas that experienced suburban development was associated with increasing emissions while population growth in the developed urban core was associated with stable emissions. Four state-of-the-art global-scale emission inventories also have a nonlinear relationship with population density across the city; however, in contrast to our observations, they all have nearly constant emissions over time. Our results indicate that decadal scale changes in urban CO2 emissions are detectable through monitoring networks and constitute a valuable approach to evaluate emission inventories and studies of urban carbon cycles.

The Southern Ocean plays a critical role in the global climate system by mediating atmosphere–ocean partitioning of heat and carbon dioxide. However, Earth system models are demonstrably deficient in the Southern Ocean, leading to large uncertainties in future air–sea CO2 flux projections under climate warming and incomplete interpretations of natural variability on interannual to geologic time scales. Here, we describe a recent aircraft observational campaign, the O2/N2 Ratio and CO2 Airborne Southern Ocean (ORCAS) study, which collected measurements over the Southern Ocean during January and February 2016. The primary research objective of the ORCAS campaign was to improve observational constraints on the seasonal exchange of atmospheric carbon dioxide and oxygen with the Southern Ocean. The campaign also included measurements of anthropogenic and marine biogenic reactive gases; high-resolution, hyperspectral ocean color imaging of the ocean surface; and microphysical data relevant for understanding and modeling cloud processes. In each of these components of the ORCAS project, the campaign has significantly expanded the amount of observational data available for this remote region. Ongoing research based on these observations will contribute to advancing our understanding of this climatically important system across a range of topics including carbon cycling, atmospheric chemistry and transport, and cloud physics. This article presents an overview of the scientific and methodological aspects of the ORCAS project and highlights early findings.

Despite the need for researchers to understand terrestrial biospheric carbon fluxes to account for carbon cycle feedbacks and predict future CO2 concentrations, knowledge of these fluxes at the regional scale remains poor. This is particularly true in mountainous areas, where complex meteorology and lack of observations lead to large uncertainties in carbon fluxes. Yet mountainous regions are often where significant forest cover and biomass are found – i.e., areas that have the potential to serve as carbon sinks. As CO2 observations are carried out in mountainous areas, it is imperative that they are properly interpreted to yield information about carbon fluxes. In this paper, we present CO2 observations at 3 sites in the mountains of the Western U.S., along with atmospheric simulations that attempt to extract information about biospheric carbon fluxes from the CO2 observations, with emphasis on the observed and simulated diurnal cycles of CO2. We show that atmospheric models can systematically simulate the wrong diurnal cycle and significantly misinterpret the CO2 observations, due to erroneous atmospheric flows as a result of terrain that is misrepresented in the model. This problem depends on the selected vertical level in the model and are exacerbated as the spatial resolution is degraded, and our results indicate that a fine grid spacing of ~ 4 km or less may be needed to simulate a realistic diurnal cycle of CO2 for sites on top of the steep mountains examined here in the American Rockies. In the absence of higher resolution models, we recommend coarse-scale models to focus on assimilating afternoon CO2 observations on mountaintop sites over the continent to avoid misrepresentations of nocturnal transport and influence.

We present two new products from near-infrared Greenhouse Gases Observing Satellite (GOSAT) observations: lowermost tropospheric (LMT, from 0 to 2.5 km) and upper tropospheric–stratospheric (U, above 2.5 km) carbon dioxide partial column mixing ratios. We compare these new products to aircraft profiles and remote surface flask measurements and find that the seasonal and year-to-year variations in the new partial column mixing ratios significantly improve upon the Atmospheric CO2 Observations from Space (ACOS) and GOSAT (ACOS-GOSAT) initial guess and/or a priori, with distinct patterns in the LMT and U seasonal cycles that match validation data. For land monthly averages, we find errors of 1.9, 0.7, and 0.8 ppm for retrieved GOSAT LMT, U, and XCO2; for ocean monthly averages, we find errors of 0.7, 0.5, and 0.5 ppm for retrieved GOSAT LMT, U, and XCO2. In the southern hemispheric biomass burning season, the new partial columns show similar patterns to MODIS fire maps and MOPITT multispectral CO for both vertical levels, despite a flat ACOS-GOSAT prior, and a CO–CO2 emission factor comparable to published values. The difference of LMT and U, useful for evaluation of model transport error, has also been validated with a monthly average error of 0.8 (1.4) ppm for ocean (land). LMT is more locally influenced than U, meaning that local fluxes can now be better separated from CO2 transported from far away.

A regional atmospheric inversion method has been developed to determine the spatial and temporal distribution of CO2 sinks and sources across New Zealand for 2011–2013. This approach infers net air–sea and air–land CO2 fluxes from measurement records, using back-trajectory simulations from the Numerical Atmospheric dispersion Modelling Environment (NAME) Lagrangian dispersion model, driven by meteorology from the New Zealand Limited Area Model (NZLAM) weather prediction model. The inversion uses in situ measurements from two fixed sites, Baring Head on the southern tip of New Zealand's North Island (41.408° S, 174.871° E) and Lauder from the central South Island (45.038° S, 169.684° E), and ship board data from monthly cruises between Japan, New Zealand, and Australia. A range of scenarios is used to assess the sensitivity of the inversion method to underlying assumptions and to ensure robustness of the results. The results indicate a strong seasonal cycle in terrestrial land fluxes from the South Island of New Zealand, especially in western regions covered by indigenous forest, suggesting higher photosynthetic and respiratory activity than is evident in the current a priori land process model. On the annual scale, the terrestrial biosphere in New Zealand is estimated to be a net CO2 sink, removing 98 (±37) Tg CO2 yr−1 from the atmosphere on average during 2011–2013. This sink is much larger than the reported 27 Tg CO2 yr−1 from the national inventory for the same time period. The difference can be partially reconciled when factors related to forest and agricultural management and exports, fossil fuel emission estimates, hydrologic fluxes, and soil carbon change are considered, but some differences are likely to remain. Baseline uncertainty, model transport uncertainty, and limited sensitivity to the northern half of the North Island are the main contributors to flux uncertainty.

The Surface Ocean CO2 NETwork (SOCONET) and atmospheric Marine Boundary Layer (MBL) CO2 measurements from ships and buoys focus on the operational aspects of measurements of CO2 in both the ocean surface and atmospheric MBLs. The goal is to provide accurate pCO2 data to within 2 micro atmosphere (μatm) for surface ocean and 0.2 parts per million (ppm) for MBL measurements following rigorous best practices, calibration and intercomparison procedures. Platforms and data will be tracked in near real-time and final quality-controlled data will be provided to the community within a year. The network, involving partners worldwide, will aid in production of important products such as maps of monthly resolved surface ocean CO2 and air-sea CO2 flux measurements. These products and other derivatives using surface ocean and MBL CO2 data, such as surface ocean pH maps and MBL CO2 maps, will be of high value for policy assessments and socio-economic decisions regarding the role of the ocean in sequestering anthropogenic CO2 and how this uptake is impacting ocean health by ocean acidification. SOCONET has an open ocean emphasis but will work with regional (coastal) networks. It will liaise with intergovernmental science organizations such as Global Atmosphere Watch (GAW), and the joint committee for and ocean and marine meteorology (JCOMM). Here we describe the details of this emerging network and its proposed operations and practices RW, AS, LB, DP, JT, NB, TT, RF, KO’B, and KT were supported by the NOAA office of Oceanic and Atmospheric Research, including the Ocean Observations and Monitoring Division (OOMD), funding reference #100007298 and PMEL contribution #4893. AO and SL were supported by the Norwegian Research Council (ICOS-Norway 245927). MT acknowledges support from the United States National Science Foundation grant OCE-1840868 to the Scientific Committee on Oceanic Research (SCOR, United States). US was supported by the European AtlantOS project (Grant Agreement #633211), RINGO project (Grant Agreement #730944), the United Kingdom NERC SONATA project (Grant No. NE/P021417/1), and RAGNARoCC project (Grant No. NE/K002473/1). PP was supported by the NERC SONATA project. MH was partly supported by the German Federal Ministry of Education and Research (grant no. 01LK1224I; ICOS-D). BT was supported by the Australia’s Integrated Marine Observing System. NCAR was sponsored by the United States National Science Foundation SI

We present observations of CHBr3, CH2Br2, CH3I, CHClBr2, and CHBrCl2 from the Trace Gas Organic Analyzer (TOGA) during the O2/N2 Ratio and CO2 Airborne Southern Ocean (ORCAS) study and the 2nd Atmospheric Tomography mission (ATom-2), in January and February of 2016 and 2017. We also use CH3Br from the University of Miami Advanced Whole Air Sampler (AWAS) on ORCAS and from the UC Irvine Whole Air Sampler (WAS) on ATom-2. We compare our observations with simulations from the Community Atmosphere Model with Chemistry (CAM-Chem). We report regional enrichment ratios of CHBr3 and CH2Br2 to O2 of 0.19 ± 0.01, and 0.07 ± 0.004 pmol : mol, poleward of 60° S between 180° W and 55° W, and of 0.32 ± 0.02, 0.07 ± 0.004 pmol : mol over the Patagonian Shelf, between 40° S and 55° S and between 70° W and 55° W where we also report enrichment ratios of CH3I to O2 of 0.38 ± 0.03 pmol : mol and of CH2ClBr2 to O2 of 0.19 ± 0.04 pmol: mol. Using the Stochastic Time-Inverted Lagrangian Transport (STILT) particle dispersion model, we use correlations between halogenated hydrocarbon mixing ratios and the upwind influences of chlorophyll a, sea ice, solar radiation, and dissolved organic material to investigate previously hypothesized sources of halogenated volatile organic compounds (HVOCs) in the southern high latitudes. Our results are consistent with a biogenic regional source of CHBr3, and both non-biological and biological sources of CH3I over these regions, but do not corroborate a regional sea-ice source of HVOCs in January and February. Based on these relationships, we estimate the average two-month (Jan.-Feb.) emissions poleward of 60° S between 180° W and 55° W of CHBr3, CH2Br2, CH3I, and CHClBr2 to be 91 ± 8, 31 ± 17, 35 ± 29, and 11 ± 4 pmol m−2 hr−1, and regional emissions of these gases over the Patagonian Shelf to be 329 ± 23, 69 ± 5, 392 ± 32, 24 ± 4 pmol m−2 hr−1 respectively.

Despite its importance to the climate system, the ocean meridional heat transport is still poorly quantified. We identify a strong link between the northern hemisphere deficit in atmospheric potential oxygen (APO = O $$_2$$ + 1.1 $$\times$$ CO $$_2$$ ) and the asymmetry in meridional heat transport between northern and southern hemispheres. The recent aircraft observations from the HIPPO campaign reveal a northern APO deficit in the tropospheric column of $$-$$ 10.4 $$\pm$$ 1.0 per meg, double the value at the surface and more representative of large-scale air–sea fluxes. The global northward ocean heat transport asymmetry necessary to explain the observed APO deficit is about 0.7–1.1 PW, which corresponds to the upper range of estimates from hydrographic sections and atmospheric reanalyses.

Observed seasonal cycles in atmospheric potential oxygen (APO ~ O2 + 1.1 CO2) were used to evaluate eight ocean biogeochemistry models from the Coupled Model Intercomparison Project (CMIP5). Model APO seasonal cycles were computed from the CMIP5 air-sea O2 and CO2 fluxes and compared to observations at three Southern Hemisphere monitoring sites. Four of the models captured either the observed APO seasonal amplitude or phasing relatively well, while the other four did not. Many models had an unrealistic seasonal phasing or amplitude of the CO2 flux, which in turn influenced APO. By 2100 under RCP8.5, the models projected little change in the O2 component of APO but large changes in the seasonality of the CO2 component associated with ocean acidification. The models with poorer performance on present-day APO tended to project larger net carbon uptake in the Southern Ocean, both today and in 2100.

Monitoring the terrestrial carbon cycle for responses to disturbances, caused for example by extreme climate events and insect outbreaks, has the potential to provide early warnings about ecosystem change. However, our capability to detect these carbon balance responses by atmospheric CO2 monitoring remains unknown despite sub-ppm comparability of many well-calibrated CO2 measurement sites. Here, this study explores how accurately atmospheric CO2 and transport models can detect imposed carbon flux anomalies against a background terrestrial flux. Air mass back trajectories from three CO2 monitoring stations in the central U.S. Rocky Mountains for one year (2008) were computationally simulated. To simulate reduced CO2 uptake, a constant +0.2 µmol C m−1 s−2 anomaly was added to all surface fluxes within perturbation domains of varying size. A spatially and temporally uniform 10°×10° +0.2 µmol C m−2 s−1 flux anomaly (+6 Tg C m−1) was detectable above a comprehensive model-data mismatch detection threshold in a large majority of months at each site, but only when the perturbation was located in the central Mountain West. The intensity of the perturbation and its area were important to detection, but the effect of area declined exponentially with increasing source-to-station distance. To further evaluate response, a more realistic spatiotemporally varying drought extracted from a dynamic global vegetation model with a monthly varying perturbation area (1°×1° to 5°×5°) and higher peak intensity (+0.8 µmol C m−2 s−1) was applied. Detectability of excess CO2 from this experiment by the nearest CO2 site (Utah) was similar to detectability of the largest (10°×10°) uniform perturbation. These experiments demonstrate disturbance and drought related carbon-cycle perturbations do create a discernible impact on the composite signal of atmospheric CO2 if sufficiently proximal to a measurement station.

We have compared a suite of recent global CO2 atmospheric inversion results to independent airborne observations and to each other, to assess their dependence on differences in northern extratropical vertical transport and to identify some of the drivers of model spread. We evaluate posterior CO2 concentration profiles against observations from the High-Performance Instrumented Airborne Platform for Environmental Research (HIAPER) Pole-to-Pole Observations (HIPPO) aircraft campaigns over the mid Pacific in 2009–2011. Although the models differ in inverse approaches, assimilated observations, prior fluxes, and transport models, their latitudinal distributions of land fluxes have converged significantly since the Atmospheric Carbon Cycle Inversion Intercomparison (TransCom3) and the REgional Carbon Cycle Assessment and Processes (RECCAP) projects, with model spread reduced by 80 % since TransCom3 and 70 % since RECCAP. Most modelled CO2 fields agree reasonably well with the HIPPO observations, in particular for annual mean vertical gradients in the northern hemisphere. Northern hemisphere vertical mixing no longer appears to be a dominant driver of northern versus tropical annual flux differences. Our newer suite of models still gives modest northern extratropical land uptake and near neutral tropical land uptake for 2009–2011, thus implying a continued strong uptake in intact tropical forests given estimates of emissions from deforestation. The results from these models for other time periods (2004–2014, 2001–2004, 1992–1996), and re-evaluation of the TransCom3 Level 2 and RECCAP results confirms that tropical land carbon fluxes including deforestation have been near neutral for several decades. However, models still have large disagreements on ocean-land partitioning, and this is influenced by differences in prescribed fossil fuel emissions and is associated with differences in retrieved atmospheric growth rate. The fossil fuel and the atmospheric growth rate terms have been thought to be the best-known terms in the global carbon budget, but we show that they dominate the model spread at the largest scales and currently limit our ability to assess regional scale terrestrial fluxes and ocean-land partitioning from the model ensemble.

Measurements of atmospheric CO2 concentration provide a tight constraint on the sum of the land and ocean sinks. This constraint has been combined with estimates of ocean carbon flux and riverine transport of carbon from land to oceans to isolate the land sink. Uncertainties in the ocean and river fluxes therefore translate into uncertainties in the land sink. Here, we introduce a heat-based constraint on the latitudinal distribution of ocean and river carbon fluxes, and reassess the partition between ocean, river and land in the tropics, and in the southern and northern extra-tropics. We show that the ocean overturning circulation and biological pump tightly link the ocean transports of heat and carbon between hemispheres. Using this coupling between heat and carbon, we derive ocean and river carbon fluxes compatible with observational constraints on heat transport. This heat-based constraint requires a 20–100% stronger ocean and river carbon transport from the Northern Hemisphere to the Southern Hemisphere than existing estimates, and supports an upward revision of the global riverine carbon flux from 0.45 to 0.78 PgC yr−1. These systematic biases in existing ocean/river carbon fluxes redistribute up to 40% of the carbon sink between northern, tropical and southern land ecosystems. As a consequence, the magnitude of both the southern land source and the northern land sink may have to be substantially reduced. Terrestrial carbon sources in the Southern Hemisphere and sinks in the Northern Hemisphere may be smaller than thought, according to a recalculation that accounts for the oceanic redistribution of carbon.

We present a 13 year (2002–2015) semimonthly time series of the partial pressure of CO2 in surface water (pCO2surf) and other carbonate system parameters from the Drake Passage. This record shows a clear increase in the magnitude of the sea-air pCO2 gradient, indicating strengthening of the CO2 sink in agreement with recent large-scale analyses of the world oceans. The rate of increase in pCO2surf north of the Antarctic Polar Front (APF) is similar to the atmospheric pCO2 (pCO2atm) trend, whereas the pCO2surf increase south of the APF is slower than the pCO2atm trend. The high-frequency surface observations indicate that an absence of a winter increase in total CO2 (TCO2) and cooling summer sea surface temperatures are largely responsible for increasing CO2 uptake south of the APF. Muted winter trends in surface TCO2 also provide temporary stability to the carbonate system that is already close to undersaturation with respect to aragonite.

In remote regions such as the open Southern Ocean, satellite observations often provide the only available tool with which to evaluate large-scale biogeochemical processes. However, these observations need to be carefully evaluated with in situ measurements. With an average of 20 crossings per year from 2002 to 2011, the Drake Passage Time-series (DPT) represents one of the most complete datasets of biogeochemical measurements in the open Southern Ocean. This dataset offers a unique opportunity to validate satellite-based productivity algorithms and to improve understanding of the role of this region in the global carbon cycle. Net community production (NCP) was estimated using discrete measurements of total dissolved inorganic carbon (TCO2) and phosphate ( PO 4 3 − ), and high-frequency underway measurements of the partial pressure of carbon dioxide in the surface ocean (pCO2surf) from the DPT, combined with estimates of gas exchange, Ekman transport, wind stress curl, and vertical entrainment. We estimate annual NCP using seasonal PO 4 3 − ( NCP PO 4 3 − ) and TCO2 ( NCP TCO 2 ) budgets of 1.2±0.7 and 1.6±0.4 mol C m−2 yr−1, respectively. Budget terms for gas exchange, entrainment, and advective supply indicate that a closed system seasonal-drawdown approach that does not consider additional terms may underestimate NCP in this region by nearly 35%. NCP estimates are compared to satellite algorithms commonly used to estimate both net primary production (NPP) and organic carbon export. Budget-based NCP approaches indicate high rates of NCP during austral spring with little additional NCP over austral summer. In contrast, satellite approaches suggest a more gradual increase and decline in NCP rates over the growing season with approximately 40% of NCP accumulating during austral summer.

INTRODUCTION The Orbiting Carbon Observatory-2 (OCO-2) is NASA’s first satellite designed to measure atmospheric carbon dioxide (CO 2 ) with the precision, resolution, and coverage necessary to quantify regional carbon sources and sinks. OCO-2 launched on 2 July 2014, and during the first 2 years of its operation, a major El Niño occurred: the 2015–2016 El Niño, which was one of the strongest events ever recorded. El Niño and its cold counterpart La Niña (collectively known as the El Niño–Southern Oscillation or ENSO) are the dominant modes of tropical climate variability. ENSO originates in the tropical Pacific Ocean but spurs a variety of anomalous weather patterns around the globe. Not surprisingly, it also leaves an imprint on the global carbon cycle. Understanding the magnitude and phasing of the ENSO-CO 2 relationship has important implications for improving the predictability of carbon-climate feedbacks. The high-density observations from NASA’s OCO-2 mission, coupled with surface ocean CO 2 measurements from NOAA buoys, have provided us with a unique data set to track the atmospheric CO 2 concentrations and unravel the timing of the response of the ocean and the terrestrial carbon cycle during the 2015–2016 El Niño. RATIONALE During strong El Niño events, there is an overall increase in global atmospheric CO 2 concentrations. This increase is predominantly due to the response of the terrestrial carbon cycle to El Niño–induced changes in weather patterns. But along with the terrestrial component, the tropical Pacific Ocean also plays an important role. Typically, the tropical Pacific Ocean is a source of CO 2 to the atmosphere due to equatorial upwelling that brings CO 2 -rich water from the interior ocean to the surface. During El Niño, this equatorial upwelling is suppressed in the eastern and the central Pacific Ocean, reducing the supply of CO 2 to the surface. If CO 2 fluxes were to remain constant elsewhere, this reduction in ocean-to-atmosphere CO 2 fluxes should contribute to a slowdown in the growth of atmospheric CO 2 . This hypothesis cannot be verified, however, without large-scale CO 2 observations over the tropical Pacific Ocean. RESULTS OCO-2 observations confirm that the tropical Pacific Ocean played an early and important role in the response of atmospheric CO 2 concentrations to the 2015–2016 El Niño. By analyzing trends in the time series of atmospheric CO 2 , we see clear evidence of an initial decrease in atmospheric CO 2 concentrations over the tropical Pacific Ocean, specifically during the early stages of the El Niño event (March through July 2015). Atmospheric CO 2 concentration anomalies suggest a flux reduction of 26 to 54% that is validated by the NOAA Tropical Atmosphere Ocean (TAO) mooring CO 2 data. Both the OCO-2 and TAO data further show that the reduction in ocean-to-atmosphere fluxes is spatially variable and has strong gradients across the tropical Pacific Ocean. During the later stages of the El Niño (August 2015 and later), the OCO-2 observations register a rise in atmospheric CO 2 concentrations. We attribute this increase to the response from the terrestrial component of the carbon cycle—a combination of reduction in biospheric uptake of CO 2 over pan-tropical regions and an enhancement in biomass burning emissions over Southeast Asia and Indonesia. The net impact of the 2015–2016 El Niño event on the global carbon cycle is an increase in atmospheric CO 2 concentrations, which would likely be larger if it were not for the reduction in outgassing from the ocean. CONCLUSION The strong El Niño event of 2015–2016 provided us with an opportunity to study how the global carbon cycle responds to a change in the physical climate system. Space-based observations of atmospheric CO 2 , such as from OCO-2, allow us to observe and monitor the temporal sequence of El Niño–induced changes in CO 2 concentrations. Disentangling the timing of the ocean and terrestrial responses is the first step toward interpreting their relative contribution to the global atmospheric CO 2 growth rate, and thereby understanding the sensitivity of the carbon cycle to climate forcing on interannual to decadal time scales. NASA’s carbon sleuth tracks the influence of El Niño on atmospheric CO 2 . The tropical Pacific Ocean, the center of action during an El Niño event, is shown in cross section. Warm ocean surface temperatures are shown in red, cooler waters in blue. The Niño 3.4 region, which scientists use to study the El Niño, is denoted by yellow dashed lines. As a result of OCO-2’s global coverage and 16-day repeat cycle, it flies over the entire region every few days, keeping tabs on the changes in atmospheric CO 2 concentration.

We present an evaluation of aircraft observations of the carbon and greenhouse gases CO2, CH4, N2O, and CO using a direct-absorption pulsed quantum cascade laser spectrometer (QCLS) operated during the HIPPO and CalNex airborne experiments. The QCLS made continuous 1 Hz measurements with 1σ Allan precisions of 20, 0.5, 0.09, and 0.15 ppb for CO2, CH4, N2O, and CO, respectively, over > 500 flight hours on 79 research flights. The QCLS measurements are compared to two vacuum ultraviolet (VUV) CO instruments (CalNex and HIPPO), a cavity ring-down spectrometer (CRDS) measuring CO2 and CH4 (CalNex), two broadband non-dispersive infrared (NDIR) spectrometers measuring CO2 (HIPPO), two onboard gas chromatographs measuring a variety of chemical species including CH4, N2O, and CO (HIPPO), and various flask-based measurements of all four species. QCLS measurements are tied to NOAA and WMO standards using an in-flight calibration system, and mean differences when compared to NOAA CCG flask data over the 59 HIPPO research flights were 100, 1, 1, and 2 ppb for CO2, CH4, N2O, and CO, respectively. The details of the end-to-end calibration procedures and the data quality assurance and quality control (QA/QC) are presented. Specifically, we discuss our practices for the traceability of standards given uncertainties in calibration cylinders, isotopic and surface effects for the long-lived greenhouse gas tracers, interpolation techniques for in-flight calibrations, and the effects of instrument linearity on retrieved mole fractions.

Fossil fuel combustion has increased atmospheric CO2 by ≈ 115 µmol mol−1 since 1750 and decreased its carbon isotope composition (δ13C) by 1.7–2‰ (the 13C Suess effect). Because carbon is stored in the terrestrial biosphere for decades and longer, the δ13C of CO2 released by terrestrial ecosystems is expected to differ from the δ13C of CO2 assimilated by land plants during photosynthesis. This isotopic difference between land-atmosphere respiration (δR) and photosynthetic assimilation (δA) fluxes gives rise to the 13C land disequilibrium (D). Contemporary understanding suggests that over annual and longer time scales, D is determined primarily by the Suess effect, and thus, D is generally positive (δR > δA). A 7 year record of biosphere-atmosphere carbon exchange was used to evaluate the seasonality of δA and δR, and the 13C land disequilibrium, in a subalpine conifer forest. A novel isotopic mixing model was employed to determine the δ13C of net land-atmosphere exchange during day and night and combined with tower-based flux observations to assess δA and δR. The disequilibrium varied seasonally and when flux-weighted was opposite in sign than expected from the Suess effect (D = −0.75 ± 0.21‰ or −0.88 ± 0.10‰ depending on method). Seasonality in D appeared to be driven by photosynthetic discrimination (Δcanopy) responding to environmental factors. Possible explanations for negative D include (1) changes in Δcanopy over decades as CO2 and temperature have risen, and/or (2) post-photosynthetic fractionation processes leading to sequestration of isotopically enriched carbon in long-lived pools like wood and soil.

“The amount of knowledge about our earth and the climate system that has been gained from sustained measurements of atmospheric CO2 and other gases is immeasurable, yet these programmes are required to justify themselves as hypothesis-driven experiments every 3 years to funding agencies with oscillating budgets and priorities.“

Observations of methyl chloroform combined with an atmospheric transport model predict a Northern to Southern Hemisphere hydroxyl ratio of slightly less than 1, whereas commonly used atmospheric chemistry models predict ratios 15–45% higher. The hydroxyl radical is an important atmospheric oxidant, but our knowledge of its global distribution remains imprecise, with estimates for the ratio of Northern Hemisphere to Southern Hemisphere hydroxyl radical concentration varying from 0.85 to 1.4. These authors use a three-dimensional chemistry-transport model that has been well validated for interhemispheric transport using sulphur hexafluoride measurements, to obtain an interhemispheric hydroxyl radical ratio of 0.97±0.12. This information can help improve our understanding of the fate of atmospheric pollutants and greenhouse gases. The hydroxyl radical (OH) is a key oxidant involved in the removal of air pollutants and greenhouse gases from the atmosphere1,2,3. The ratio of Northern Hemispheric to Southern Hemispheric (NH/SH) OH concentration is important for our understanding of emission estimates of atmospheric species such as nitrogen oxides and methane4,5,6. It remains poorly constrained, however, with a range of estimates from 0.85 to 1.4 (refs 4, 7,8,9,10). Here we determine the NH/SH ratio of OH with the help of methyl chloroform data (a proxy for OH concentrations) and an atmospheric transport model that accurately describes interhemispheric transport and modelled emissions. We find that for the years 2004–2011 the model predicts an annual mean NH–SH gradient of methyl chloroform that is a tight linear function of the modelled NH/SH ratio in annual mean OH. We estimate a NH/SH OH ratio of 0.97 ± 0.12 during this time period by optimizing global total emissions and mean OH abundance to fit methyl chloroform data from two surface-measurement networks and aircraft campaigns11,12,13. Our findings suggest that top-down emission estimates of reactive species such as nitrogen oxides in key emitting countries in the NH that are based on a NH/SH OH ratio larger than 1 may be overestimated.

We present one of the first estimates of the global distribution of CO2 surface fluxes using total column CO2 measurements retrieved by the SRON-KIT RemoTeC algorithm from the Greenhouse gases Observing SATellite (GOSAT). We derive optimized fluxes from June 2009 to December 2010. We estimate fluxes from surface CO2 measurements to use as baselines for comparing GOSAT data-derived fluxes. Assimilating only GOSAT data, we can reproduce the observed CO2 time series at surface and TCCON sites in the tropics and the northern extra-tropics. In contrast, in the southern extra-tropics GOSAT XCO2 leads to enhanced seasonal cycle amplitudes compared to independent measurements, and we identify it as the result of a land–sea bias in our GOSAT XCO2 retrievals. A bias correction in the form of a global offset between GOSAT land and sea pixels in a joint inversion of satellite and surface measurements of CO2 yields plausible global flux estimates which are more tightly constrained than in an inversion using surface CO2 data alone. We show that assimilating the bias-corrected GOSAT data on top of surface CO2 data (a) reduces the estimated global land sink of CO2, and (b) shifts the terrestrial net uptake of carbon from the tropics to the extra-tropics. It is concluded that while GOSAT total column CO2 provide useful constraints for source–sink inversions, small spatiotemporal biases – beyond what can be detected using current validation techniques – have serious consequences for optimized fluxes, even aggregated over continental scales.