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Abstract. Marine diazotrophs convert dinitrogen (N2) gas intobioavailable nitrogen (N), supporting life in the global ocean. In 2012, thefirst version of the global oceanic diazotroph database (version 1) waspublished. Here, we present an updated version of the database (version 2),significantly increasing the number of in situ diazotrophic measurements from13 565 to 55 286. Data points for N2 fixation rates, diazotrophic cellabundance, and nifH gene copy abundance have increased by 184 %, 86 %, and809 %, respectively. Version 2 includes two new data sheets for the nifH genecopy abundance of non-cyanobacterial diazotrophs and cell-specific N2fixation rates. The measurements of N2 fixation rates approximatelyfollow a log-normal distribution in both version 1 and version 2. However,version 2 considerably extends both the left and right tails of thedistribution. Consequently, when estimating global oceanic N2 fixationrates using the geometric means of different ocean basins, version 1 andversion 2 yield similar rates (43–57 versus 45–63 Tg N yr−1; rangesbased on one geometric standard error). In contrast, when using arithmeticmeans, version 2 suggests a significantly higher rate of 223±30 Tg N yr−1 (mean ± standard error; same hereafter) compared to version 1(74±7 Tg N yr−1). Specifically, substantial rate increases areestimated for the South Pacific Ocean (88±23 versus 20±2 Tg N yr−1), primarily driven by measurements in the southwestern subtropics,and for the North Atlantic Ocean (40±9 versus 10±2 Tg N yr−1). Moreover, version 2 estimates the N2 fixation rate in theIndian Ocean to be 35±14 Tg N yr−1, which could not be estimatedusing version 1 due to limited data availability. Furthermore, a comparisonof N2 fixation rates obtained through different measurement methods atthe same months, locations, and depths reveals that the conventional15N2 bubble method yields lower rates in 69 % cases compared tothe new 15N2 dissolution method. This updated version of thedatabase can facilitate future studies in marine ecology andbiogeochemistry. The database is stored at the Figshare repository(https://doi.org/10.6084/m9.figshare.21677687; Shao etal., 2022).

We assess scientific evidence that has emerged since the U.S. Environmental Protection Agency's 2009 Endangerment Finding for six well-mixed greenhouse gases and find that this new evidence lends increased support to the conclusion that these gases pose a danger to public health and welfare. Newly available evidence about a wide range of observed and projected impacts strengthens the association between the risk of some of these impacts and anthropogenic climate change, indicates that some impacts or combinations of impacts have the potential to be more severe than previously understood, and identifies substantial risk of additional impacts through processes and pathways not considered in the Endangerment Finding.

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is an interdisciplinary investigation to improve understanding of Earth's ocean ecosystem-aerosol-cloud system. Specific overarching science objectives for NAAMES are to (1) characterize plankton ecosystem properties during primary phases of the annual cycle and their dependence on environmental forcings, (2) determine how these phases interact to recreate each year the conditions for an annual plankton bloom, and (3) resolve how remote marine aerosols and boundary layer clouds are influenced by plankton ecosystems. Four NAAMES field campaigns were conducted in the western subarctic Atlantic between November 2015 and April 2018, with each campaign targeting specific seasonal events in the annual plankton cycle. A broad diversity of measurements were collected during each campaign, including ship, aircraft, autonomous float and drifter, and satellite observations. Here, we present an overview of NAAMES science motives, experimental design, and measurements. We then briefly describe conditions and accomplishments during each of the four field campaigns and provide information on how to access NAAMES data. The intent of this manuscript is to familiarize the broad scientific community with NAAMES and to provide a common reference overview of the project for upcoming publications.

Using the Community Earth System Model, we explore the role of human land use and land cover change (LULCC) in modifying the terrestrial carbon budget in simulations forced by Representative Concentration Pathway 8.5, extended to year 2300. Overall, conversion of land (e.g., from forest to croplands via deforestation) results in a model-estimated, cumulative carbon loss of 490 Pg C between 1850 and 2300, larger than the 230 Pg C loss of carbon caused by climate change over this same interval. The LULCC carbon loss is a combination of a direct loss at the time of conversion and an indirect loss from the reduction of potential terrestrial carbon sinks. Approximately 40% of the carbon loss associated with LULCC in the simulations arises from direct human modification of the land surface; the remaining 60% is an indirect consequence of the loss of potential natural carbon sinks. Because of the multicentury carbon cycle legacy of current land use decisions, a globally averaged amplification factor of 2.6 must be applied to 2015 land use carbon losses to adjust for indirect effects. This estimate is 30% higher when considering the carbon cycle evolution after 2100. Most of the terrestrial uptake of anthropogenic carbon in the model occurs from the influence of rising atmospheric CO2 on photosynthesis in trees, and thus, model-projected carbon feedbacks are especially sensitive to deforestation.

This study characterized ocean biological carbon pump metrics in the second iteration of the REgional Carbon Cycle Assessment and Processes (RECCAP2) project. The analysis here focused on comparisons of global and biome‐scale regional patterns in particulate organic carbon (POC) production and sinking flux from the RECCAP2 ocean biogeochemical model ensemble against observational products derived from satellite remote sensing, sediment traps, and geochemical methods. There was generally good model‐data agreement in mean large‐scale spatial patterns, but with substantial spread across the model ensemble and observational products. The global‐integrated, model ensemble‐mean export production, taken as the sinking POC flux at 100 m (6.08 ± 1.17 Pg C yr−1), and export ratio defined as sinking flux divided by net primary production (0.154 ± 0.026) both fell at the lower end of observational estimates. Comparison with observational constraints also suggested that the model ensemble may have underestimated regional biological CO2 drawdown and air‐sea CO2 flux in high productivity regions. Reasonable model‐data agreement was found for global‐integrated, ensemble‐mean sinking POC flux into the deep ocean at 1,000 m (0.65 ± 0.24 Pg C yr−1) and the transfer efficiency defined as flux at 1,000 m divided by flux at 100 m (0.122 ± 0.041), with both variables exhibiting considerable regional variability. The RECCAP2 analysis presents standard ocean biological carbon pump metrics for assessing biogeochemical model skill, metrics that are crucial for further modeling efforts to resolve remaining uncertainties involving system‐level interactions between ocean physics and biogeochemistry. Plain Language Summary: Phytoplankton in the surface ocean create each year an amount of organic carbon approximately equivalent to all the annual photosynthesis by plants on land. A small fraction of this newly formed organic carbon is exported below the surface layer, and an even smaller amount makes it all the way to the deep ocean. The transport of organic carbon to the sub‐surface ocean, called the biological carbon pump, influences the global‐scale distributions of ocean nutrients, oxygen, and inorganic carbon as well as the amount of carbon dioxide in the atmosphere. The global rates and geographic patterns of photosynthesis and carbon flux out of the surface ocean have previously been constructed from ship measurements and satellite remote sensing. Here, we compare these observation‐based estimates to a suite of three‐dimensional numerical ocean models and find broadly similar results. The model simulations also capture aspects of the biological carbon pump deeper in the water column, where there are fewer direct constraints from field observations. Our comparison of observations and simulations identifies some deficiencies in the models that should be corrected in order to better simulate climate change impacts on the biological carbon pump. Key Points: Global‐scale, ocean biogeochemical simulations are compared with observation‐based estimates of the marine biological carbon pumpA multi‐model ensemble exhibits good agreement with observation‐based metrics for carbon export flux and transfer efficiencyBased on identified model‐observation and inter‐model differences, we provide guidance for future model evaluations and development [ABSTRACT FROM AUTHOR]

Version 1 of the Community Earth SystemModel, in the configurationwhere its full carbon cycle is enabled, is introduced and documented. In this configuration, the terrestrial biogeochemical model, which includes carbon-nitrogen dynamics and is present in earlier model versions, is coupled to an ocean biogeochemical model and atmospheric CO2 tracers. The authors provide a description of the model, detail how preindustrial-control and twentieth-century experiments were initialized and forced, and examine the behavior of the carbon cycle in those experiments. They examine how sea- and land-to-air CO2 fluxes contribute to the increase of atmospheric CO2 in the twentieth century, analyze how atmospheric CO2 and its surface fluxes vary on interannual time scales, including how they respond to ENSO, and describe the seasonal cycle of atmospheric CO2 and its surface fluxes. While the model broadly reproduces observed aspects of the carbon cycle, there are several notable biases, including having too large of an increase in atmospheric CO2 over the twentieth century and too small of a seasonal cycle of atmospheric CO2 in the Northern Hemisphere. The biases are related to a weak response of the carbon cycle to climatic variations on interannual and seasonal time scales and to twentieth-century anthropogenic forcings, including rising CO2, land-use change, and atmospheric deposition of nitrogen.

The response of the carbon cycle in prognostic Earth system models (ESMs) contributes significant uncertainty to projections of global climate change. Quantifying contributions of known drivers of interannual variability in the growth rate of atmospheric carbon dioxide (CO2) is important for improving the representation of terrestrial ecosystem processes in these ESMs. Several recent studies have identified the temperature dependence of tropical net ecosystem exchange (NEE) as a primary driver of this variability by analyzing a single, globally averaged time series of CO2 anomalies. Here we examined how the temporal evolution of CO2 in different latitude bands may be used to separate contributions from temperature stress, drought stress, and fire emissions to CO2 variability. We developed atmospheric CO2 patterns from each of these mechanisms during 1997-2011 using an atmospheric transport model. NEE responses to temperature, NEE responses to drought, and fire emissions all contributed significantly to CO2 variability in each latitude band, suggesting that no single mechanism was the dominant driver. We found that the sum of drought and fire contributions to CO2 variability exceeded direct NEE responses to temperature in both the Northern and Southern Hemispheres. Additional sensitivity tests revealed that these contributions are masked by temporal and spatial smoothing of CO2 observations. Accounting for fires, the sensitivity of tropical NEE to temperature stress decreased by 25% to 2.9 ± 0.4 Pg C yr-1 K-1. These results underscore the need for accurate attribution of the drivers of CO2 variability prior to using contemporary observations to constrain long-term ESM responses.

Interannual variability (IAV) in the atmospheric CO2 growth rate is caused by variation in the balance between uptake by land and ocean and accumulation of anthropogenic emissions in the atmosphere. While variations in terrestrial fluxes are thought to drive most of the observed atmospheric CO2 IAV, the ability to characterize ocean impacts has been limited by the fact that most sites in the surface CO2 monitoring network are located on coasts or islands or within the continental interior. NASA's Orbiting Carbon-Observatory 2 (OCO-2) mission has observed the atmospheric total column carbon dioxide mole fraction (XCO2) from space since September 2014. With a near-global coverage, this dataset provides a first opportunity to directly observe IAV in atmospheric CO2 over remote ocean regions. We assess the impact of ocean flux IAV on the OCO-2 record using atmospheric transport simulations with underlying gridded air-sea CO2 fluxes from observation-based products. We use three observation-based products to bracket the likely range of ocean air-sea flux contributions to XCO2 variability (over both land and ocean) within the GEOS-Chem atmospheric transport model. We find that the magnitude of XCO2 IAV generated by the whole ocean is between 0.08-0.12 ppm throughout the world. Depending on location and flux product, between 20-80% of the IAV in the simulations is caused by IAV in air-sea CO2 fluxes, with the remainder due to IAV in atmospheric winds, which modulate the atmospheric gradients that arise from climatological ocean fluxes. The Southern Hemisphere mid-latitudes and low-latitudes are the dominant ocean regions in generating the XCO2 IAV globally. The simulation results based on all three flux products show that even within the Northern Hemisphere atmosphere, Southern Hemisphere ocean fluxes are the dominant source of variability in XCO2. Nevertheless, the small magnitude of the air-sea flux impacts on XCO2 presents a substantial challenge for detection of oceandriven IAV from OCO-2. Although the IAV amplitude arising from ocean fluxes and transport is 20 to 50% of the total observed XCO2 IAV amplitude of 0.4 to 1.6 ppm in the Southern Hemisphere and the tropics, ocean-driven IAV represents only 10% of the observed amplitude in the Northern Hemisphere. We find that for all three products, the simulated ocean-driven XCO2 IAV is weakly anticorrelated with OCO-2 observations, although these correlations are not statistically significant (p>0.05), suggesting that even over ocean basins, terrestrial IAV obscures the ocean signal. [ABSTRACT FROM AUTHOR]

Here we analyze the impact of projected climate change on plankton ecology in all major ocean biomes over the 21st century, using a multidecade (1880–2090) experiment conducted with the Community Climate System Model (CCSM-3.1) coupled ocean-atmosphere-land-sea ice model. The climate response differs fundamentally in the Northern and Southern Hemispheres for diatom and small phytoplankton biomass and consequently for total biomass, primary, and export production. Increasing vertical stratification in the Northern Hemisphere oceans decreases the nutrient supply to the ocean surface. Resulting decreases in diatom and small phytoplankton biomass together with a relative shift from diatoms to small phytoplankton in the Northern Hemisphere result in decreases in the total primary and export production and export ratio, and a shift to a more oligotrophic, more efficiently recycled, lower biomass euphotic layer. By contrast, temperature and stratification increases are smaller in the Southern compared to the Northern Hemisphere. Additionally, a southward shift and increase in strength of the Southern Ocean westerlies act against increasing temperature and freshwater fluxes to destratify the water-column. The wind-driven, poleward shift in the Southern Ocean subpolar-subtropical boundary results in a poleward shift and increase in the frontal diatom bloom. This boundary shift, localized increases in iron supply, and the direct impact of warming temperatures on phytoplankton growth result in diatom increases in the Southern Hemisphere. An increase in diatoms and decrease in small phytoplankton partly compensate such that while total production and the efficiency of organic matter export to the deep ocean increase, total Southern Hemisphere biomass does not change substantially. The impact of ecological shifts on the global carbon cycle is complex and varies across ecological biomes, with Northern and Southern Hemisphere effects on the biological production and export partially compensating. The net result of climate change is a small Northern Hemisphere-driven decrease in total primary production and efficiency of organic matter export to the deep ocean.

The authors compare Community Earth System Model results to marine observations for the 1990s and examine climate change impacts on biogeochemistry at the end of the twenty-first century under two future scenarios (Representative Concentration Pathways RCP4.5 and RCP8.5). Late-twentieth-century seasonally varying mixed layer depths are generally within 10 m of observations, with a Southern Ocean shallow bias. Surface nutrient and chlorophyll concentrations exhibit positive biases at low latitudes and negative biases at high latitudes. The volume of the oxygen minimum zones is overestimated.The impacts of climate change on biogeochemistry have similar spatial patterns under RCP4.5 and RCP8.5, but perturbation magnitudes are larger under RCP8.5. Increasing stratification leads to weaker nutrient entrainment and decreased primary and export production (>30% over large areas). The global-scale decreases in primary and export production scale linearly with the increases in mean sea surface temperature. There are production increases in the high nitrate, low chlorophyll (HNLC) regions, driven by lateral iron inputs from adjacent areas. The increased HNLC export partially compensates for the reductions in non-HNLC waters (~25% offset). Stabilizing greenhouse gas emissions and climate by the end of this century (as in RCP4.5) will minimize the changes to nutrient cycling and primary production in the oceans. In contrast, continued increasing emission of CO2 (as in RCP8.5) will lead to reduced productivity and significant modifications to ocean circulation and biogeochemistry by the end of this century, with more drastic changes beyond the year 2100 as the climate continues to rapidly warm.

Ocean carbon uptake and storage simulated by the Community Earth System Model, version 1–Biogeochemistry [CESM1(BGC)], is described and compared to observations. Fully coupled and ocean-ice configurations are examined; both capture many aspects of the spatial structure and seasonality of surface carbon fields. Nearly ubiquitous negative biases in surface alkalinity result from the prescribed carbonate dissolution profile. The modeled sea–air CO2 fluxes match observationally based estimates over much of the ocean; significant deviations appear in the Southern Ocean. Surface ocean pCO2 is biased high in the subantarctic and low in the sea ice zone. Formation of the water masses dominating anthropogenic CO2 (Cant) uptake in the Southern Hemisphere is weak in the model, leading to significant negative biases in Cant and chlorofluorocarbon (CFC) storage at intermediate depths. Column inventories of Cant appear too high, by contrast, in the North Atlantic. In spite of the positive bias, this marks an improvement over prior versions of the model, which underestimated North Atlantic uptake. The change in behavior is attributable to a new parameterization of density-driven overflows. CESM1(BGC) provides a relatively robust representation of the ocean–carbon cycle response to climate variability. Statistical metrics of modeled interannual variability in sea–air CO2 fluxes compare reasonably well to observationally based estimates. The carbon cycle response to key modes of climate variability is basically similar in the coupled and forced ocean-ice models; however, the two differ in regional detail and in the strength of teleconnections.

Changes in atmospheric CO2 variability during the twenty-first century may provide insight about ecosystem responses to climate change and have implications for the design of carbon monitoring programs. This paper describes changes in the three-dimensional structure of atmospheric CO2 for several representative concentration pathways (RCPs 4.5 and 8.5) using the Community Earth System Model–Biogeochemistry (CESM1-BGC). CO2 simulated for the historical period was first compared to surface, aircraft, and column observations. In a second step, the evolution of spatial and temporal gradients during the twenty-first century was examined. The mean annual cycle in atmospheric CO2 was underestimated for the historical period throughout the Northern Hemisphere, suggesting that the growing season net flux in the Community Land Model (the land component of CESM) was too weak. Consistent with weak summer drawdown in Northern Hemisphere high latitudes, simulated CO2 showed correspondingly weak north–south and vertical gradients during the summer. In the simulations of the twenty-first century, CESM predicted increases in the mean annual cycle of atmospheric CO2 and larger horizontal gradients. Not only did the mean north–south gradient increase due to fossil fuel emissions, but east–west contrasts in CO2 also strengthened because of changing patterns in fossil fuel emissions and terrestrial carbon exchange. In the RCP8.5 simulation, where CO2 increased to 1150 ppm by 2100, the CESM predicted increases in interannual variability in the Northern Hemisphere midlatitudes of up to 60% relative to present variability for time series filtered with a 2–10-yr bandpass. Such an increase in variability may impact detection of changing surface fluxes from atmospheric observations.

This study used an ocean general circulation model to simulate the marine iron cycle in an investigation of how simulated distributions of weak iron-binding ligands would be expected to control dissolved iron concentrations in the ocean, with a particular focus on deep ocean waters. The distribution of apparent oxygen utilization was used as a proxy for humic substances that have recently been hypothesized to account for the bulk of weak iron-binding ligands in seawater. Compared to simulations using a conventional approach with homogeneous ligand distributions, the simulations that incorporated spatially variable ligand concentrations exhibited substantial improvement in the simulation of global dissolved iron distributions as revealed by comparisons with available field data. The improved skill of the simulations resulted largely because the spatially variable ligand distributions led to a more reasonable basin-scale variation of the residence time of iron when present at high concentrations. The model results, in conjunction with evidence from recent field studies, suggest that humic substances play an important role in the iron cycle in the ocean.

The performance of 36 models (22 ocean color models and 14 biogeochemical ocean circulation models (BOGCMs)) that estimate depth-integrated marine net primary productivity (NPP) was assessed by comparing their output to in situ 14C data at the Bermuda Atlantic Time series Study (BATS) and the Hawaii Ocean Time series (HOT) over nearly two decades. Specifically, skill was assessed based on the models' ability to estimate the observed mean, variability, and trends of NPP. At both sites, more than 90% of the models underestimated mean NPP, with the average bias of the BOGCMs being nearly twice that of the ocean color models. However, the difference in overall skill between the best BOGCM and the best ocean color model at each site was not significant. Between 1989 and 2007, in situ NPP at BATS and HOT increased by an average of nearly 2% per year and was positively correlated to the North Pacific Gyre Oscillation index. The majority of ocean color models produced in situ NPP trends that were closer to the observed trends when chlorophyll-a was derived from high-performance liquid chromatography (HPLC), rather than fluorometric or SeaWiFS data. However, this was a function of time such that average trend magnitude was more accurately estimated over longer time periods. Among BOGCMs, only two individual models successfully produced an increasing NPP trend (one model at each site). We caution against the use of models to assess multiannual changes in NPP over short time periods. Ocean color model estimates of NPP trends could improve if more high quality HPLC chlorophyll-a time series were available.

Efforts to control climate change require the stabilization of atmospheric CO 2 concentrations. This can only be achieved through a drastic reduction of global CO 2 emissions. Yet fossil fuel emissions increased by 29% between 2000 and 2008, in conjunction with increased contributions from emerging economies, from the production and international trade of goods and services, and from the use of coal as a fuel source. In contrast, emissions from land-use changes were nearly constant. Between 1959 and 2008, 43% of each year's CO 2 emissions remained in the atmosphere on average; the rest was absorbed by carbon sinks on land and in the oceans. In the past 50 years, the fraction of CO 2 emissions that remains in the atmosphere each year has likely increased, from about 40% to 45%, and models suggest that this trend was caused by a decrease in the uptake of CO 2 by the carbon sinks in response to climate change and variability. Changes in the CO 2 sinks are highly uncertain, but they could have a significant influence on future atmospheric CO 2 levels. It is therefore crucial to reduce the uncertainties. © 2009 Macmillan Publishers Limited. All rights reserved.

With representation of the global carbon cycle becoming increasingly complex in climate models, it is important to develop ways to quantitatively evaluate model performance against in situ and remote sensing observations. Here we present a systematic framework, the Carbon-LAnd Model Intercomparison Project (C-LAMP), for assessing terrestrial biogeochemistry models coupled to climate models using observations that span a wide range of temporal and spatial scales. As an example of the value of such comparisons, we used this framework to evaluate two biogeochemistry models that are integrated within the Community Climate System Model (CCSM) -Carnegie-Ames-Stanford Approach′ (CASA′) and carbon-nitrogen (CN). Both models underestimated the magnitude of net carbon uptake during the growing season in temperate and boreal forest ecosystems, based on comparison with atmospheric CO 2 measurements and eddy covariance measurements of net ecosystem exchange. Comparison with MODerate Resolution Imaging Spectroradiometer (MODIS) measurements show that this low bias in model fluxes was caused, at least in part, by 1-3 month delays in the timing of maximum leaf area. In the tropics, the models overestimated carbon storage in woody biomass based on comparison with datasets from the Amazon. Reducing this model bias will probably weaken the sensitivity of terrestrial carbon fluxes to both atmospheric CO2 and climate. Global carbon sinks during the 1990s differed by a factor of two (2.4PgCyr-1 for CASA′ vs. 1.2PgCyr-1 for CN), with fluxes from both models compatible with the atmospheric budget given uncertainties in other terms. The models captured some of the timing of interannual global terrestrial carbon exchange during 1988-2004 based on comparison with atmospheric inversion results from TRANSCOM (r =0.66 for CASA′ and r =0.73 for CN). Adding (CASA′) or improving (CN) the representation of deforestation fires may further increase agreement with the atmospheric record. Information from C-LAMP has enhanced model performance within CCSM and serves as a benchmark for future development. We propose that an open source, community-wide platform for model-data intercomparison is needed to speed model development and to strengthen ties between modeling and measurement communities. Important next steps include the design and analysis of land use change simulations (in both uncoupled and coupled modes), and the entrainment of additional ecological and earth system observations. Model results from C-LAMP are publicly available on the Earth System Grid. © 2009 Blackwell Publishing Ltd.

We present results from transient sensitivity studies with the Biogeochemical Elemental Cycling (BEC) ocean model to increasing anthropogenic atmospheric inorganic nitrogen (N) and soluble iron (Fe) deposition over the industrial era. Elevated N deposition results from fossil fuel combustion and agriculture, and elevated soluble Fe deposition results from increased atmospheric processing in the presence of anthropogenic pollutants and soluble Fe from combustion sources. Simulations with increasing Fe and increasing Fe and N inputs raised simulated marine nitrogen fixation, with the majority of the increase in the subtropical North and South Pacific, and raised primary production and export in the high-nutrient low-chlorophyll (HNLC) regions. Increasing N inputs alone elevated small phytoplankton and diatom production, resulting in increased phosphorus (P) and Fe limitation for diazotrophs, hence reducing nitrogen fixation (∼6%). Globally, the simulated primary production, sinking particulate organic carbon (POC) export. and atmospheric CO2 uptake were highest under combined increase in Fe and N inputs compared to preindustrial control. Our results suggest that increasing combustion iron sources and aerosol Fe solubility along with atmospheric anthropogenic nitrogen deposition are perturbing marine biogeochemical cycling and could partially explain the observed trend toward increased P limitation at station ALOHA in the subtropical North Pacific. Excess inorganic nitrogen ([NO3 −] + [NH4 +] − 16[PO4 3−]) distributions may offer useful insights for understanding changing ocean circulation and biogeochemistry.

We quantify the mechanisms governing interannual variability in the global, upper-ocean inorganic carbon system using a hindcast simulation (1979-2004) of an ecosystem-biogeochemistry model forced with time-evolving atmospheric physics and dust deposition. We analyze the variability of three key, interrelated metrics-air-sea CO2 flux, surface-water carbon dioxide partial pressure pCO2, and upper-ocean dissolved inorganic carbon (DIC) inventory-presenting for each metric global spatial maps of the root mean square (rms) of anomalies from a model monthly climatology. The contribution of specific driving factors is diagnosed using Taylor expansions and linear regression analysis. The major regions of variability occur in the Southern Ocean, tropical Indo-Pacific, and Northern Hemisphere temperate and subpolar latitudes. Ocean circulation is the dominant factor driving variability over most of the ocean, modulating surface dissolved inorganic carbon that in turn alters surface-water pCO2 and air-sea CO2 flux variability (global integrated anomaly rms of 0.34 Pg C yr-1). Biological export and thermal solubility effects partially damp circulation-driven pCO2 variability in the tropics, while in the subtropics, thermal solubility contributes positively to surface-water pCO2 and air-sea CO2 flux variability. Gas transfer and net freshwater inputs induce variability in the air-sea CO2 flux in some specific regions. A component of air-sea CO2 flux variability (global integrated anomaly rms of 0.14 Pg C yr-1) arises from variations in biological export production induced by variations in atmospheric iron deposition downwind of dust source regions. Beginning in the mid-1990s, reduced global dust deposition generates increased air-sea CO2 outgassing in the Southern Ocean, consistent with trends derived from atmospheric CO2 inversions. © 2008 Elsevier Ltd.