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The extended multilinear regression method is used to determine the uptake and storage of anthropogenic carbon in the Atlantic Ocean based on repeat occupations of four cruises from 1989 to 2014 (A16, A20, A22, and A10), with an emphasis on the 2003–2014 period. The results show a significant increase in basin-wide anthropogenic carbon storage in the North Atlantic, which absorbed 4.4 ± 0.9 Pg C decade−1 from 2003 to 2014 compared to 1.9 ± 0.4 Pg C decade−1 for the 1989–2003 period. This decadal variability is attributed to changing ventilation patterns associated with the North Atlantic Oscillation and increasing release of anthropogenic carbon into the atmosphere. There are small changes in the uptake rate of CO2 in the South Atlantic for these time periods (3.7 ± 0.8 Pg C decade−1 versus 3.2 ± 0.7 Pg C decade−1). Several eddies are identified containing ~20% more anthropogenic carbon than the surrounding waters in the South Atlantic demonstrating the importance of eddies in transporting anthropogenic carbon. The uptake of carbon results in a decrease in pH of ~0.0021 ± 0.0007 year−1 for surface waters during the last 10 years, in line with the atmospheric increase in CO2.

High quality total inorganic carbon (CT) measurements made in the major ocean basins as part of the Joint Global Ocean Flux Study (JGOFS), the National Oceanic and Atmospheric Administration/Ocean Atmosphere Carbon Exchange Study (NOAA/OACES), and the Department of Energy/World Ocean Circulation Experiment (DOE/WOCE) programs are related to sea surface temperature (SST) and nitrate (NO3−). A simple two-parameter function with SST and NO3− of the form NCT = a + b SST + c SST2 + d NO3− fits salinity (S)-normalized surface CT (NCT = CT × 35/S) data for different parts of the oceans within an area-weighted error of ±7 μmol kg−1 (1σ). Estimated values of NCT using the derived algorithms with NO3− and SST are compared with values calculated from the surface partial pressure of CO2 (pCO2sw) [Takahashi et al.,1997] and total alkalinity (AT) [Millero et al., 1998] fields using thermodynamic models. Comparisons of the estimated values of NCT with measurements not used to derive the same algorithms, and comparisons with the values calculated from global AT and pCO2sw fields, give a realistic uncertainty of ±15 μmol kg−1 in estimated CT. The derived correlations of NCT with SST and NO3− presented here make it possible to estimate surface CT over the ocean from climatological SST, S, and NO3− fields.

[1] Based on measurements from the WOCE/JGOFS global CO2 survey, the CLIVAR/CO2 Repeat Hydrography Program and the Canadian Line P survey, we have observed an average decrease of 0.34% yr−1 in the saturation state of surface seawater in the Pacific Ocean with respect to aragonite and calcite. The upward migrations of the aragonite and calcite saturation horizons, averaging about 1 to 2 m yr−1, are the direct result of the uptake of anthropogenic CO2 by the oceans and regional changes in circulation and biogeochemical processes. The shoaling of the saturation horizon is regionally variable, with more rapid shoaling in the South Pacific where there is a larger uptake of anthropogenic CO2. In some locations, particularly in the North Pacific Subtropical Gyre and in the California Current, the decadal changes in circulation can be the dominant factor in controlling the migration of the saturation horizon. If CO2 emissions continue as projected over the rest of this century, the resulting changes in the marine carbonate system would mean that many coral reef systems in the Pacific would no longer be able to sustain a sufficiently high rate of calcification to maintain the viability of these ecosystems as a whole, and these changes perhaps could seriously impact the thousands of marine species that depend on them for survival.

[1] The North Atlantic Ocean accounts for about 25% of the global oceanic anthropogenic carbon sink. This basin experiences significant interannual variability primarily driven by the North Atlantic Oscillation (NAO). A suite of biogeochemical model simulations is used to analyze the impact of interannual variability on the uptake and storage of contemporary and anthropogenic carbon (Canthro) in the North Atlantic Ocean. Greater winter mixing during positive NAO years results in increased mode water formation and subsequent increases in subtropical and subpolar Canthro inventories. Our analysis suggests that changes in mode water Canthro inventories are primarily due to changes in water mass volumes driven by variations in water mass transformation rates rather than local air-sea CO2 exchange. This suggests that a significant portion of anthropogenic carbon found in the ocean interior may be derived from surface waters advected into water formation regions rather than from local gas exchange. Therefore, changes in climate modes, such as the NAO, may alter the residence time of anthropogenic carbon in the ocean by altering the rate of water mass transformation. In addition, interannual variability in Canthro storage increases the difficulty of Canthro detection and attribution through hydrographic observations, which are limited by sparse sampling of subsurface waters in time and space.

[1] A common approach for estimating the oceanic uptake of anthropogenic carbon dioxide (Canthro) depends on the linear approximation of oceanic dissolved inorganic carbon (DIC) from a suite of physical and biological ocean parameters. The extended multiple linear regression (eMLR) method assumes that baseline correlations and the resulting residual fields will remain constant with time even under the influence of secular climate changes. The validity of these assumptions over the 21st century is tested using a coupled carbon-climate model. Findings demonstrate that the influence of both changing climate and changing chemistry beyond 2–4 decades invalidates the assumption that the residual fields will remain constant resulting in significant errors in the eMLR estimate of Canthro. This study determines that the eMLR method is unable to describe Canthro uptake for a sampling interval of greater than 30 years if the error is to remain below 20% for many regions in the Southern Ocean, Atlantic Ocean, and western Pacific Ocean. These results suggest that, for many regions of the ocean basins, hydrographic field investigations have to be repeated at approximately decadal timescales in order to accurately predict the uptake of Canthro by the ocean if the eMLR method is used.

[1] Recent studies based on ocean and atmospheric carbon dioxide (CO2) observations, suggesting that the ocean carbon uptake has been reduced, may help explain the increase in the fraction of anthropogenic CO2 emissions that remain in the atmosphere. Is it a response to climate change or a signal of ocean natural variability or both? Regional process analyses are needed to follow the ocean carbon uptake and to enable better attributions of the observed changes. Here, we describe the evolution of the surface ocean CO2 fugacity (fCO2oc) over the period 1993–2008 in the North Atlantic subpolar gyre (NASPG). This analysis is based primarily on observations of dissolved inorganic carbon (DIC) and total alkalinity (TA) conducted at different seasons in the NASPG between Iceland and Canada. The fCO2oc trends based on DIC and TA data are also compared with direct fCO2 measurements obtained between 2003 and 2007 in the same region. During winters 1993–2003, the fCO2oc growth rate was 3.7 (±0.6) μatm yr−1, higher than in the atmosphere, 1.8 (±0.1) μatm yr−1. This translates to a reduction of the ocean carbon uptake primarily explained by sea surface warming, up to 0.24 (±0.04) °C yr−1. This warming is a consequence of advection of warm water northward from the North Atlantic into the Irminger basin, which occurred as the North Atlantic Oscillation (NAO) index moved into a negative phase in winter 1995/1996. In winter 2001–2008, the fCO2oc rise was particularly fast, between 5.8 (±1.1) and 7.2 (±1.3) μatm yr−1 depending on the region, more than twice the atmospheric growth rate of 2.1 (±0.2) μatm yr−1, and in the winter of 2007–2008 the area was supersaturated with CO2. As opposed to the 1990s, this appears to be almost entirely due to changes in seawater carbonate chemistry, the combination of increasing DIC and decreasing of TA. The rapid fCO2oc increase was not only driven by regional uptake of anthropogenic CO2 but was also likely controlled by a recent increase in convective processes-vertical mixing in the NASPG and cannot be directly associated with NAO variability. The fCO2oc increase observed in 2001–2008 leads to a significant drop in pH of −0.069 (±0.007) decade−1.

Observational studies report a rapid decline of ocean CO2 uptake in the temperate North Atlantic during the last decade. We analyze these findings using ocean physical‐biological numerical simulations forced with interannually varying atmospheric conditions for the period 1979–2004. In the simulations, surface ocean water mass properties and CO2 system variables exhibit substantial multiannual variability on sub‐basin scales in response to wind‐driven reorganization in ocean circulation and surface warming/cooling. The simulated temporal evolution of the ocean CO2 system is broadly consistent with reported observational trends and is influenced substantially by the phase of the North Atlantic Oscillation (NAO). Many of the observational estimates cover a period after 1995 of mostly negative or weakly positive NAO conditions, which are characterized in the simulations by reduced North Atlantic Current transport of subtropical waters into the eastern basin and by a decline in CO2 uptake. We suggest therefore that air‐sea CO2 uptake may rebound in the eastern temperate North Atlantic during future periods of more positive NAO, similar to the patterns found in our model for the sustained positive NAO period in the early 1990s. Thus, our analysis indicates that the recent rapid shifts in CO2 flux reflect decadal perturbations superimposed on more gradual secular trends. The simulations highlight the need for long‐term ocean carbon observations and modeling to fully resolve multiannual variability, which can obscure detection of the long‐term changes associated with anthropogenic CO2 uptake and climate change.

[1] The 14CO2 released into the stratosphere during bomb testing in the early 1960s provides a global constraint on air-sea gas exchange of soluble atmospheric gases like CO2. Using the most complete database of dissolved inorganic radiocarbon, DI14C, available to date and a suite of ocean general circulation models in an inverse mode we recalculate the ocean inventory of bomb-produced DI14C in the global ocean and confirm that there is a 25% decrease from previous estimates using older DI14C data sets. Additionally, we find a 33% lower globally averaged gas transfer velocity for CO2 compared to previous estimates (Wanninkhof, 1992) using the NCEP/NCAR Reanalysis 1 1954–2000 where the global mean winds are 6.9 m s−1. Unlike some earlier ocean radiocarbon studies, the implied gas transfer velocity finally closes the gap between small-scale deliberate tracer studies and global-scale estimates. Additionally, the total inventory of bomb-produced radiocarbon in the ocean is now in agreement with global budgets based on radiocarbon measurements made in the stratosphere and troposphere. Using the implied relationship between wind speed and gas transfer velocity ks = 0.27〈u102〉(Sc/660)−0.5 and standard partial pressure difference climatology of CO2 we obtain an net air-sea flux estimate of 1.3 ± 0.5 PgCyr−1 for 1995. After accounting for the carbon transferred from rivers to the deep ocean, our estimate of oceanic uptake (1.8 ± 0.5 PgCyr−1) compares well with estimates based on ocean inventories, ocean transport inversions using ocean concentration data, and model simulations.

[1] During the 1990s, ocean sampling expeditions were carried out as part of the World Ocean Circulation Experiment (WOCE), the Joint Global Ocean Flux Study (JGOFS), and the Ocean Atmosphere Carbon Exchange Study (OACES). Subsequently, a group of U.S. scientists synthesized the data into easily usable and readily available products. This collaboration is known as the Global Ocean Data Analysis Project (GLODAP). Results were merged into a common format data set, segregated by ocean. For comparison purposes, each ocean data set includes a small number of high-quality historical cruises. The data were subjected to rigorous quality control procedures to eliminate systematic data measurement biases. The calibrated 1990s data were used to estimate anthropogenic CO2, potential alkalinity, CFC watermass ages, CFC partial pressure, bomb-produced radiocarbon, and natural radiocarbon. These quantities were merged into the measured data files. The data were used to produce objectively gridded property maps at a 1° resolution on 33 depth surfaces chosen to match existing climatologies for temperature, salinity, oxygen, and nutrients. The mapped fields are interpreted as an annual mean distribution in spite of the inaccuracy in that assumption. Both the calibrated data and the gridded products are available from the Carbon Dioxide Information Analysis Center. Here we describe the important details of the data treatment and the mapping procedure, and present summary quantities and integrals for the various parameters.