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Interannual anomalies in the sea-air carbon dioxide (CO2 ) exchange have been estimated from surface-ocean CO2 partial pressure measurements. Available data are sufficient to constrain these anomalies in large parts of the tropical and North Pacific and in the North Atlantic, in some areas covering the period from the mid 1980s to 2011. Global interannual variability is estimated as about 0.31 Pg C yr-1 (temporal standard deviation 1993-2008). The tropical Pacific accounts for a large fraction of this global variability, closely tied to El Niño-Southern Oscillation (ENSO). Anomalies occur more than 6 months later in the east than in the west. The estimated amplitude and ENSO response are roughly consistent with independent information from atmospheric oxygen data. This both supports the variability estimated from surface-ocean carbon data and demonstrates the potential of the atmospheric oxygen signal to constrain ocean biogeochemical processes. The ocean variability estimated from surface-ocean carbon data can be used to improve land CO2 flux estimates from atmospheric inversions.

The Atlantic Ocean is one of the most important sinks for atmospheric carbon dioxide (CO2), but this sink has been shown to vary substantially in time. Here we use surface ocean CO2 observations to estimate this sink and the temporal variability from 1998 through 2007 in the Atlantic Ocean. We benefit from (i) a continuous improvement of the observations, i.e. the Surface Ocean CO2 Atlas (SOCAT) v1.5 database and (ii) a newly developed technique to interpolate the observations in space and time. In particular, we use a two-step neural network approach to reconstruct basin-wide monthly maps of the sea surface partial pressure of CO2 (pCO2) at a resolution of 1° × 1°. From those, we compute the air–sea CO2 flux maps using a standard gas exchange parameterization and high-resolution wind speeds. The neural networks fit the observed pCO2 data with a root mean square error (RMSE) of about 10 μatm and with almost no bias. A check against independent time-series data and new data from SOCAT v2 reveals a larger RMSE of 22.8 μatm for the entire Atlantic Ocean, which decreases to 16.3 μatm for data south of 40° N. We estimate a decadal mean uptake flux of −0.45 ± 0.15 Pg C yr−1 for the Atlantic between 44° S and 79° N, representing the sum of a strong uptake north of 18° N (−0.39 ± 0.10 Pg C yr−1), outgassing in the tropics (18° S–18° N, 0.11 ± 0.07 Pg C yr−1), and uptake in the subtropical/temperate South Atlantic south of 18° S (−0.16 ± 0.06 Pg C yr−1), consistent with recent studies. The strongest seasonal variability of the CO2 flux occurs in the temperature-driven subtropical North Atlantic, with uptake in winter and outgassing in summer. The seasonal cycle is antiphased in the subpolar latitudes relative to the subtropics largely as a result of the biologically driven winter-to-summer drawdown of CO2. Over the 10 yr analysis period (1998 through 2007), sea surface pCO2 increased faster than that of the atmosphere in large areas poleward of 40° N, while in other regions of the North Atlantic the sea surface pCO2 increased at a slower rate, resulting in a barely changing Atlantic carbon sink north of the Equator (−0.01 ± 0.02 Pg C yr−1 decade−1). Surface ocean pCO2 increased at a slower rate relative to atmospheric CO2 over most of the Atlantic south of the Equator, leading to a substantial trend toward a stronger CO2 sink for the entire South Atlantic (−0.14 ± 0.02 Pg C yr−1 decade−1). In contrast to the 10 yr trends, the Atlantic Ocean carbon sink varies relatively little on inter-annual timescales (±0.04 Pg C yr−1; 1 σ).

Using measurements of the surface-ocean CO2 partial pressure (pCO2) and 14 different pCO2 mapping methods recently collated by the Surface Ocean pCO2 Mapping intercomparison (SOCOM) initiative, variations in regional and global sea–air CO2 fluxes are investigated. Though the available mapping methods use widely different approaches, we find relatively consistent estimates of regional pCO2 seasonality, in line with previous estimates. In terms of interannual variability (IAV), all mapping methods estimate the largest variations to occur in the eastern equatorial Pacific. Despite considerable spread in the detailed variations, mapping methods that fit the data more closely also tend to agree more closely with each other in regional averages. Encouragingly, this includes mapping methods belonging to complementary types – taking variability either directly from the pCO2 data or indirectly from driver data via regression. From a weighted ensemble average, we find an IAV amplitude of the global sea–air CO2 flux of 0.31 PgC yr-1 (standard deviation over 1992–2009), which is larger than simulated by biogeochemical process models. From a decadal perspective, the global ocean CO2 uptake is estimated to have gradually increased since about 2000, with little decadal change prior to that. The weighted mean net global ocean CO2 sink estimated by the SOCOM ensemble is -1.75 PgC yr-1 (1992–2009), consistent within uncertainties with estimates from ocean-interior carbon data or atmospheric oxygen trends.

Carbon dioxide (CO2) is, next to water vapour, considered to be the most important natural greenhouse gas on Earth. Rapidly rising atmospheric CO2 concentrations caused by human actions such as fossil fuel burning, land-use change or cement production over the past 250 years have given cause for concern that changes in Earth's climate system may progress at a much faster pace and larger extent than during the past 20 000 years. Investigating global carbon cycle pathways and finding suitable adaptation and mitigation strategies has, therefore, become of major concern in many research fields. The oceans have a key role in regulating atmospheric CO2 concentrations and currently take up about 25% of annual anthropogenic carbon emissions to the atmosphere. Questions that yet need to be answered are what the carbon uptake kinetics of the oceans will be in the future and how the increase in oceanic carbon inventory will affect its ecosystems and their services. This requires comprehensive investigations, including high-quality ocean carbon measurements on different spatial and temporal scales, the management of data in sophisticated databases, the application of Earth system models to provide future projections for given emission scenarios as well as a global synthesis and outreach to policy makers. In this paper, the current understanding of the ocean as an important carbon sink is reviewed with respect to these topics. Emphasis is placed on the complex interplay of different physical, chemical and biological processes that yield both positive and negative air–sea flux values for natural and anthropogenic CO2 as well as on increased CO2 (uptake) as the regulating force of the radiative warming of the atmosphere and the gradual acidification of the oceans. Major future ocean carbon challenges in the fields of ocean observations, modelling and process research as well as the relevance of other biogeochemical cycles and greenhouse gases are discussed.

Coccolithophores are a key functional group in terms of the pelagic production of calcium carbonate (calcite), although their contribution to shelf sea biogeochemistry, and how this relates to environmental conditions, is poorly constrained. Measurements of calcite production (CP) and coccolithophore abundance were made on the north-west European shelf to examine trends in coccolithophore calcification along natural gradients of carbonate chemistry, macronutrient availability and plankton composition. Similar measurements were also made in three bioassay experiments where nutrient (nitrate, phosphate) and pCO2 levels were manipulated. Nanoflagellates (< 10 μm) dominated chlorophyll biomass and primary production (PP) at all but one sampling site, with CP ranging from 0.6 to 9.6 mmol C m−2 d−1. High CP and coccolithophore abundance occurred in a diatom bloom in fully mixed waters off Heligoland, but not in two distinct coccolithophore blooms in the central North Sea and Western English Channel. Coccolithophore abundance and CP showed no correlation with nutrient concentrations or ratios, while significant (p < 0.01) correlations between CP, cell-specific calcification (cell-CF) and irradiance in the water column highlighted how light availability exerts a strong control on pelagic CP. In the experimental bioassays, Emiliania-huxleyi-dominated coccolithophore communities in shelf waters (northern North Sea, Norwegian Trench) showed a strong response in terms of CP to combined nitrate and phosphate addition, mediated by changes in cell-CF and growth rates. In contrast, an offshore diverse coccolithophore community (Bay of Biscay) showed no response to nutrient addition, while light availability or mortality may have been more important in controlling this community. Sharp decreases in pH and a rough halving of calcite saturation states in the bioassay experiments led to decreased CP in the Bay of Biscay and northern North Sea, but not the Norwegian Trench. These decreases in CP were related to slowed growth rates in the bioassays at elevated pCO2 (750 μatm) relative to those in the ambient treatments. The combined results from our study highlight the variable coccolithophore responses to irradiance, nutrients and carbonate chemistry in north-west European shelf waters, which are mediated by changes in growth rates, cell-CF and species composition.

As a result of ocean acidification, aragonite may become undersaturated by 2050 in the upper layers of the Southern Ocean. Analyses of sea snail specimens, extracted live from the Southern Ocean in January and February 2008, show that the shells of these organisms are already dissolving. The carbonate chemistry of the surface ocean is rapidly changing with ocean acidification, a result of human activities 1 . In the upper layers of the Southern Ocean, aragonite—a metastable form of calcium carbonate with rapid dissolution kinetics—may become undersaturated by 2050 (ref.  2 ). Aragonite undersaturation is likely to affect aragonite-shelled organisms, which can dominate surface water communities in polar regions 3 . Here we present analyses of specimens of the pteropod Limacina helicina antarctica that were extracted live from the Southern Ocean early in 2008. We sampled from the top 200 m of the water column, where aragonite saturation levels were around 1, as upwelled deep water is mixed with surface water containing anthropogenic CO 2 . Comparing the shell structure with samples from aragonite-supersaturated regions elsewhere under a scanning electron microscope, we found severe levels of shell dissolution in the undersaturated region alone. According to laboratory incubations of intact samples with a range of aragonite saturation levels, eight days of incubation in aragonite saturation levels of 0.94–1.12 produces equivalent levels of dissolution. As deep-water upwelling and CO 2 absorption by surface waters is likely to increase as a result of human activities 2 , 4 , we conclude that upper ocean regions where aragonite-shelled organisms are affected by dissolution are likely to expand.

Four carbonate system variables were measured in surface waters during a cruise aimed at investigating ocean acidification impacts traversing northwestern European shelf seas in the summer of 2011. High-resolution surface water data were collected for partial pressure of carbon dioxide (pCO2; using two independent instruments) and pH using the total pH scale (pHT), in addition to discrete measurements of total alkalinity and dissolved inorganic carbon. We thus overdetermined the carbonate system (four measured variables, two degrees of freedom), which allowed us to evaluate the level of agreement between the variables on a cruise whose main aim was not intercomparison, and thus where conditions were more representative of normal working conditions. Calculations of carbonate system variables from other measurements generally compared well with direct observations of the same variables (Pearson's correlation coefficient always greater than or equal to 0.94; mean residuals were similar to the respective accuracies of the measurements). We therefore conclude that four of the independent data sets of carbonate chemistry variables were of high quality. A diurnal cycle with a maximum amplitude of 41 μatm was observed in the difference between the pCO2 values obtained by the two independent analytical pCO2 systems, and this was partly attributed to irregular seawater flows to the equilibrator and partly to biological activity inside the seawater supply and one of the equilibrators. We discuss how these issues can be addressed to improve carbonate chemistry data quality on future research cruises.

Photosynthesis by marine phytoplankton in the Southern Ocean, and the associated uptake of carbon, is thought to be currently limited by the availability of iron 1 , 2 . One implication of this limitation is that a larger iron supply to the region in glacial times 3 could have stimulated algal photosynthesis, leading to lower concentrations of atmospheric CO 2 . Similarly, it has been proposed that artificial iron fertilization of the oceans might increase future carbon sequestration. Here we report data from a whole-ecosystem test of the iron-limitation hypothesis in the Southern Ocean 4 , which show that surface uptake of atmospheric CO 2 and uptake ratios of silica to carbon by phytoplankton were strongly influenced by nanomolar increases of iron concentration. We use these results to inform a model of global carbon and ocean nutrients, forced with atmospheric iron fluxes to the region derived from the Vostok 3 ice-core dust record. During glacial periods, predicted magnitudes and timings of atmospheric CO 2 changes match ice-core records well. At glacial terminations, the model suggests that forcing of Southern Ocean biota by iron caused the initial ∼40 p.p.m. of glacial–interglacial CO 2 change, but other mechanisms must have accounted for the remaining 40 p.p.m. increase. The experiment also confirms that modest sequestration of atmospheric CO 2 by artificial additions of iron to the Southern Ocean is in principle possible, although the period and geographical extent over which sequestration would be effective remain poorly known.

A temporally and spatially resolved estimate of the global surface-ocean CO2 partial pressure field and the sea-air CO2 flux is presented, obtained by fitting a simple data-driven diagnostic model of ocean mixed-layer biogeochemistry to surface-ocean CO2 partial pressure data from the SOCAT v1.5 database. Results include seasonal, interannual, and short-term (daily) variations. In most regions, estimated seasonality is well constrained from the data, and compares well to the widely used monthly climatology by Takahashi et al. (2009). Comparison to independent data tentatively supports the slightly higher seasonal variations in our estimates in some areas. We also fitted the diagnostic model to atmospheric CO2 data. The results of this are less robust, but in those areas where atmospheric signals are not strongly influenced by land flux variability, their seasonality is nevertheless consistent with the results based on surface-ocean data. From a comparison with an independent seasonal climatology of surface-ocean nutrient concentration, the diagnostic model is shown to capture relevant surface-ocean biogeochemical processes reasonably well. Estimated interannual variations will be presented and discussed in a companion paper.

Water column dissolved inorganic carbon and total alkalinity were measured during five hydrographic sections in the Atlantic Ocean and Drake Passage. The work was funded through the Strategic Funding Initiative of the UK's Oceans2025 programme, which ran from 2007 to 2012. The aims of this programme were to establish the regional budgets of natural and anthropogenic carbon in the North Atlantic, the South Atlantic, and the Atlantic sector of the Southern Ocean, as well as the rates of change of these budgets. This paper describes in detail the dissolved inorganic carbon and total alkalinity data collected along east–west sections at 47° N to 60° N, 24.5° N, and 24° S in the Atlantic and across two Drake Passage sections. Other hydrographic and biogeochemical parameters were measured during these sections, and relevant standard operating procedures are mentioned here. Over 95% of dissolved inorganic carbon and total alkalinity samples taken during the 24.5° N, 24° S, and the Drake Passage sections were analysed onboard and subjected to a first-level quality control addressing technical and analytical issues. Samples taken along 47° N to 60° N were analysed and subjected to quality control back in the laboratory. Complete post-cruise second-level quality control was performed using cross-over analysis with historical data in the vicinity of measurements, and data were submitted to the CLIVAR and Carbon Hydrographic Data Office (CCHDO), the Carbon Dioxide Information Analysis Center (CDIAC) and and will be included in the Global Ocean Data Analyses Project, version 2 (GLODAP 2), the upcoming update of Key et al. (2004).