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Abstract The low-noise amplification of weak microwave signals is crucial for countless protocols in quantum information processing. Quantum mechanics sets an ultimate lower limit of half a photon to the added input noise for phase-preserving amplification of narrowband signals, also known as the standard quantum limit (SQL). This limit, which is equivalent to a maximum quantum efficiency of 0.5, can be overcome by employing nondegenerate parametric amplification of broadband signals. We show that, in principle, a maximum quantum efficiency of unity can be reached. Experimentally, we find a quantum efficiency of 0.69 ± 0.02, well beyond the SQL, by employing a flux-driven Josephson parametric amplifier and broadband thermal signals. We expect that our results allow for fundamental improvements in the detection of ultraweak microwave signals.

Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere – the global carbon budget – is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and methodology to quantify the five major components of the global carbon budget and their uncertainties. CO2 emissions from fossil fuels and industry (EFF) are based on energy statistics and cement production data, respectively, while emissions from land-use change (ELUC), mainly deforestation, are based on land-cover change data and bookkeeping models. The global atmospheric CO2 concentration is measured directly and its rate of growth (GATM) is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN) and terrestrial CO2 sink (SLAND) are estimated with global process models constrained by observations. The resulting carbon budget imbalance (BIM), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the last decade available (2007–2016), EFF was 9.4 ± 0.5 GtC yr−1, ELUC 1.3 ± 0.7 GtC yr−1, GATM 4.7 ± 0.1 GtC yr−1, SOCEAN 2.4 ± 0.5 GtC yr−1, and SLAND 3.0 ± 0.8 GtC yr−1, with a budget imbalance BIM of 0.6 GtC yr−1 indicating overestimated emissions and/or underestimated sinks. For year 2016 alone, the growth in EFF was approximately zero and emissions remained at 9.9 ± 0.5 GtC yr−1. Also for 2016, ELUC was 1.3 ± 0.7 GtC yr−1, GATM was 6.1 ± 0.2 GtC yr−1, SOCEAN was 2.6 ± 0.5 GtC yr−1, and SLAND was 2.7 ± 1.0 GtC yr−1, with a small BIM of −0.3 GtC. GATM continued to be higher in 2016 compared to the past decade (2007–2016), reflecting in part the high fossil emissions and the small SLAND consistent with El Niño conditions. The global atmospheric CO2 concentration reached 402.8 ± 0.1 ppm averaged over 2016. For 2017, preliminary data for the first 6–9 months indicate a renewed growth in EFF of +2.0 % (range of 0.8 to 3.0 %) based on national emissions projections for China, USA, and India, and projections of gross domestic product (GDP) corrected for recent changes in the carbon intensity of the economy for the rest of the world. This living data update documents changes in the methods and data sets used in this new global carbon budget compared with previous publications of this data set (Le Quéré et al., 2016, 2015b, a, 2014, 2013). All results presented here can be downloaded from https://doi.org/10.18160/GCP-2017 (GCP, 2017).

We developed a battery-powered carbon dioxide (CO2) measurement system for monitoring at the summit of Mt. Fuji (3776 m a.s.l.), which experiences very low temperatures (below −20 °C) and severe environmental conditions without access to gridded electricity for 10 months (from September to June). Our measurement system used 100 batteries to run the measurement unit during these months. These batteries were charged during the 2-month summer season when gridded electricity was available, using a specially designed automatic battery-charging system. We installed this system in summer 2009 at the Mt. Fuji weather station; observations of atmospheric CO2 concentration were taken through December 2015. Measurements were never interrupted by a lack of battery power except for two cases in which lightning damaged a control board. Thus we obtained CO2 data during about 94 % of the 6-year period. Analytical performances (stability and accuracy) were better than 0.1 ppm, as tested by checking working standards and comparisons with flask sampling.Observational results showed that CO2 mole fractions at Mt. Fuji demonstrated clear seasonal variation. The trend and the variability of the CO2 growth rate observed at Mt. Fuji were very similar to those of the Mauna Loa Observatory (MLO). Seasonally, the concentration at Mt. Fuji was 2–10 ppm lower in summer and 2–12 ppm higher in winter than those at MLO. The lower concentrations at Mt. Fuji in summer are mainly attributed to episodes of air mass transport from Siberia or China, where CO2 is taken up by the terrestrial biosphere. On the other hand, the relatively higher concentrations in winter seem to reflect the high percentage of air masses originating from China or Southeast Asia during this period, which carry increased anthropogenic carbon dioxide. These results show that Mt. Fuji is not very influenced by local sources but rather by the sources and sinks over a very large region.Thus we conclude that, as this system could provide stable measurement data with relatively easy operation for 6 years at Mt. Fuji, it could be a useful monitoring technique for remote background sites elsewhere.

The Surface Ocean CO2 Atlas (SOCAT) is a synthesis of quality-controlled fCO2 (fugacity of carbon dioxide) values for the global surface oceans and coastal seas with regular updates. Version 3 of SOCAT has 14.7 million fCO2 values from 3646 data sets covering the years 1957 to 2014. This latest version has an additional 4.6 million fCO2 values relative to version 2 and extends the record from 2011 to 2014. Version 3 also significantly increases the data availability for 2005 to 2013. SOCAT has an average of approximately 1.2 million surface water fCO2 values per year for the years 2006 to 2012. Quality and documentation of the data has improved. A new feature is the data set quality control (QC) flag of E for data from alternative sensors and platforms. The accuracy of surface water fCO2 has been defined for all data set QC flags. Automated range checking has been carried out for all data sets during their upload into SOCAT. The upgrade of the interactive Data Set Viewer (previously known as the Cruise Data Viewer) allows better interrogation of the SOCAT data collection and rapid creation of high-quality figures for scientific presentations. Automated data upload has been launched for version 4 and will enable more frequent SOCAT releases in the future. High-profile scientific applications of SOCAT include quantification of the ocean sink for atmospheric carbon dioxide and its long-term variation, detection of ocean acidification, as well as evaluation of coupled-climate and ocean-only biogeochemical models. Users of SOCAT data products are urged to acknowledge the contribution of data providers, as stated in the SOCAT Fair Data Use Statement. This ESSD (Earth System Science Data) "living data" publication documents the methods and data sets used for the assembly of this new version of the SOCAT data collection and compares these with those used for earlier versions of the data collection (Pfeil et al., 2013; Sabine et al., 2013; Bakker et al., 2014). Individual data set files, included in the synthesis product, can be downloaded here: doi:10.1594/PANGAEA.849770. The gridded products are available here: doi:10.3334/CDIAC/OTG.SOCAT_V3_GRID.

The ocean has become more acidic over the last 200 years in response increasing atmospheric carbon dioxide (CO2) levels. Documenting how the ocean has changed is critical for assessing how these changes impact marine ecosystems and for the management of marine resources. Here we use present-day ocean carbon observations, from shelf and offshore waters around Australia, combined with neural network mapping of CO2, sea surface temperature, and salinity to estimate the current seasonal and regional distributions of carbonate chemistry (pH and aragonite saturation state). The observed changes in atmospheric CO2 and sea surface temperature (SST) and climatological salinity are then used to reconstruct pH and aragonite saturation state changes over the last 140 years (1870–2013). The comparison with data collected at Integrated Marine Observing System National Reference Station sites located on the shelf around Australia shows that both the mean state and seasonality in the present day are well represented, with the exception of sites such as the Great Barrier Reef. Our reconstruction predicts that since 1870 decrease in aragonite saturation state of 0.48 and of 0.09 in pH has occurred in response to increasing oceanic uptake of atmospheric CO2. Large seasonal variability in pH and aragonite saturation state occur in southwestern Australia driven by ocean dynamics (mixing) and in the Tasman Sea by seasonal warming (in the case of the aragonite saturation state). The seasonal and historical changes in aragonite saturation state and pH have different spatial patterns and suggest that the biological responses to ocean acidification are likely to be non-uniform depending on the relative sensitivity of organisms to shifts in pH and saturation state. This new historical reconstruction provides an important link to biological observations that will help to elucidate the consequences of ocean acidification.

Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and a methodology to quantify all major components of the global carbon budget, including their uncertainties, based on the combination of a range of data, algorithms, statistics, and model estimates and their interpretation by a broad scientific community. We discuss changes compared to previous estimates as well as consistency within and among components, alongside methodology and data limitations. CO2 emissions from fossil fuels and industry (EFF) are based on energy statistics and cement production data, while emissions from land-use change (ELUC), mainly deforestation, are based on combined evidence from land-cover-change data, fire activity associated with deforestation, and models. The global atmospheric CO2 concentration is measured directly and its rate of growth (GATM) is computed from the annual changes in concentration. The mean ocean CO2 sink (SOCEAN) is based on observations from the 1990s, while the annual anomalies and trends are estimated with ocean models. The variability in SOCEAN is evaluated with data products based on surveys of ocean CO2 measurements. The global residual terrestrial CO2 sink (SLAND) is estimated by the difference of the other terms of the global carbon budget and compared to results of independent dynamic global vegetation models forced by observed climate, CO2, and land-cover change (some including nitrogen–carbon interactions). We compare the mean land and ocean fluxes and their variability to estimates from three atmospheric inverse methods for three broad latitude bands. All uncertainties are reported as ±1σ, reflecting the current capacity to characterise the annual estimates of each component of the global carbon budget. For the last decade available (2005–2014), EFF was 9.0 ± 0.5 GtC yr−1, ELUC was 0.9 ± 0.5 GtC yr−1, GATM was 4.4 ± 0.1 GtC yr−1, SOCEAN was 2.6 ± 0.5 GtC yr−1, and SLAND was 3.0 ± 0.8 GtC yr−1. For the year 2014 alone, EFF grew to 9.8 ± 0.5 GtC yr−1, 0.6 % above 2013, continuing the growth trend in these emissions, albeit at a slower rate compared to the average growth of 2.2 % yr−1 that took place during 2005–2014. Also, for 2014, ELUC was 1.1 ± 0.5 GtC yr−1, GATM was 3.9 ± 0.2 GtC yr−1, SOCEAN was 2.9 ± 0.5 GtC yr−1, and SLAND was 4.1 ± 0.9 GtC yr−1. GATM was lower in 2014 compared to the past decade (2005–2014), reflecting a larger SLAND for that year. The global atmospheric CO2 concentration reached 397.15 ± 0.10 ppm averaged over 2014. For 2015, preliminary data indicate that the growth in EFF will be near or slightly below zero, with a projection of −0.6 [range of −1.6 to +0.5] %, based on national emissions projections for China and the USA, and projections of gross domestic product corrected for recent changes in the carbon intensity of the global economy for the rest of the world. From this projection of EFF and assumed constant ELUC for 2015, cumulative emissions of CO2 will reach about 555 ± 55 GtC (2035 ± 205 GtCO2) for 1870–2015, about 75 % from EFF and 25 % from ELUC. This living data update documents changes in the methods and data sets used in this new carbon budget compared with previous publications of this data set (Le Quéré et al., 2015, 2014, 2013). All observations presented here can be downloaded from the Carbon Dioxide Information Analysis Center (doi:10.3334/CDIAC/GCP_2015).

The Surface Ocean CO2 Atlas (SOCAT), an activity of the international marine carbon research community, provides access to synthesis and gridded fCO2 (fugacity of carbon dioxide) products for the surface oceans. Version 2 of SOCAT is an update of the previous release (version 1) with more data (increased from 6.3 million to 10.1 million surface water fCO2 values) and extended data coverage (from 1968–2007 to 1968–2011). The quality control criteria, while identical in both versions, have been applied more strictly in version 2 than in version 1. The SOCAT website (http://www.socat.info/) has links to quality control comments, metadata, individual data set files, and synthesis and gridded data products. Interactive online tools allow visitors to explore the richness of the data. Applications of SOCAT include process studies, quantification of the ocean carbon sink and its spatial, seasonal, year-to-year and longerterm variation, as well as initialisation or validation of ocean carbon models and coupled climate-carbon models. Data coverage Repository-References: Individual data set files and synthesis product: doi:10.1594/PANGAEA.811776 Gridded products: doi:10.3334/CDIAC/OTG.SOCAT_V2_GRID Available at: http://www.socat.info/ Coverage: 79° S to 90° N; 180° W to 180° E Location Name: Global Oceans and Coastal Seas Date/Time Start: 16 November 1968 Date/Time End: 26 December 2011

Air–sea CO2 fluxes over the Pacific Ocean are known to be characterized by coherent large-scale structures that reflect not only ocean subduction and upwelling patterns, but also the combined effects of wind-driven gas exchange and biology. On the largest scales, a large net CO2 influx into the extratropics is associated with a robust seasonal cycle, and a large net CO2 efflux from the tropics is associated with substantial interannual variability. In this work, we have synthesized estimates of the net air–sea CO2 flux from a variety of products, drawing upon a variety of approaches in three sub-basins of the Pacific Ocean, i.e., the North Pacific extratropics (18–66° N), the tropical Pacific (18° S–18° N), and the South Pacific extratropics (44.5–18° S). These approaches include those based on the measurements of CO2 partial pressure in surface seawater (pCO2sw), inversions of ocean-interior CO2 data, forward ocean biogeochemistry models embedded in the ocean general circulation models (OBGCMs), a model with assimilation of pCO2sw data, and inversions of atmospheric CO2 measurements. Long-term means, interannual variations and mean seasonal variations of the regionally integrated fluxes were compared in each of the sub-basins over the last two decades, spanning the period from 1990 through 2009. A simple average of the long-term mean fluxes obtained with surface water pCO2 diagnostics and those obtained with ocean-interior CO2 inversions are −0.47 ± 0.13 Pg C yr−1 in the North Pacific extratropics, +0.44 ± 0.14 Pg C yr−1 in the tropical Pacific, and −0.37 ± 0.08 Pg C yr−1 in the South Pacific extratropics, where positive fluxes are into the atmosphere. This suggests that approximately half of the CO2 taken up over the North and South Pacific extratropics is released back to the atmosphere from the tropical Pacific. These estimates of the regional fluxes are also supported by the estimates from OBGCMs after adding the riverine CO2 flux, i.e., −0.49 ± 0.02 Pg C yr−1 in the North Pacific extratropics, +0.41 ± 0.05 Pg C yr−1 in the tropical Pacific, and −0.39 ± 0.11 Pg C yr−1 in the South Pacific extratropics. The estimates from the atmospheric CO2 inversions show large variations amongst different inversion systems, but their median fluxes are consistent with the estimates from climatological pCO2sw data and pCO2sw diagnostics. In the South Pacific extratropics, where CO2 variations in the surface and ocean interior are severely undersampled, the difference in the air–sea CO2 flux estimates between the diagnostic models and ocean-interior CO2 inversions is larger (0.18 Pg C yr−1). The range of estimates from forward OBGCMs is also large (−0.19 to −0.72 Pg C yr−1). Regarding interannual variability of air–sea CO2 fluxes, positive and negative anomalies are evident in the tropical Pacific during the cold and warm events of the El Niño–Southern Oscillation in the estimates from pCO2sw diagnostic models and from OBGCMs. They are consistent in phase with the Southern Oscillation Index, but the peak-to-peak amplitudes tend to be higher in OBGCMs (0.40 ± 0.09 Pg C yr−1) than in the diagnostic models (0.27 ± 0.07 Pg C yr−1).

Increasing the acidity of ocean waters will directly threaten calcifying marine organisms such as reef-building scleractinian corals, and the myriad of species that rely on corals for protection and sustenance. Ocean pH has already decreased by around 0.1 pH units since the beginning of the industrial revolution, and is expected to decrease by another 0.2–0.4 pH units by 2100. This study mimicked the pre-industrial, present, and near-future levels of pCO2 using a precise control system (± 5% pCO2), to assess the impact of ocean acidification on the calcification of recently settled primary polyps of Acropora digitifera, both with and without symbionts, and adult fragments with symbionts. The increase in pCO2 of ~100 μatm between the pre-industrial period and the present had more effect on the calcification rate of adult A. digitifera than the anticipated future increases of several hundreds of micro-atmospheres of pCO2. The primary polyps with symbionts showed higher calcification rates than primary polyps without symbionts, suggesting that: (i) primary polyps housing symbionts are more tolerant to near-future ocean acidification than organisms without symbionts, and (ii) corals acquiring symbionts from the environment (i.e., broadcasting species) will be more vulnerable to ocean acidification than corals that maternally acquire symbionts.

This study uses a neural network technique to produce maps of the partial pressure of oceanic carbon dioxide (pCO2sea) in the North Pacific on a 0.25° latitude × 0.25° longitude grid from 2002 to 2008. The pCO2sea distribution was computed using a self-organizing map (SOM) originally utilized to map the pCO2sea in the North Atlantic. Four proxy parameters – sea surface temperature (SST), mixed layer depth, chlorophyll a concentration, and sea surface salinity (SSS) – are used during the training phase to enable the network to resolve the nonlinear relationships between the pCO2sea distribution and biogeochemistry of the basin. The observed pCO2sea data were obtained from an extensive dataset generated by the volunteer observation ship program operated by the National Institute for Environmental Studies (NIES). The reconstructed pCO2sea values agreed well with the pCO2sea measurements, with the root-mean-square error ranging from 17.6 μatm (for the NIES dataset used in the SOM) to 20.2 μatm (for independent dataset). We confirmed that the pCO2sea estimates could be improved by including SSS as one of the training parameters and by taking into account secular increases of pCO2sea that have tracked increases in atmospheric CO2. Estimated pCO2sea values accurately reproduced pCO2sea data at several time series locations in the North Pacific. The distributions of pCO2sea revealed by 7 yr averaged monthly pCO2sea maps were similar to Lamont-Doherty Earth Observatory pCO2sea climatology, allowing, however, for a more detailed analysis of biogeochemical conditions. The distributions of pCO2sea anomalies over the North Pacific during the winter clearly showed regional contrasts between El Niño and La Niña years related to changes of SST and vertical mixing.

As a response to public demand for a well-documented, quality controlled, publically available, global surface ocean carbon dioxide (CO2) data set, the international marine carbon science community developed the Surface Ocean CO2 Atlas (SOCAT). The first SOCAT product is a collection of 6.3 million quality controlled surface CO2 data from the global oceans and coastal seas, spanning four decades (1968–2007). The SOCAT gridded data presented here is the second data product to come from the SOCAT project. Recognizing that some groups may have trouble working with millions of measurements, the SOCAT gridded product was generated to provide a robust, regularly spaced CO2 fugacity (fCO2) product with minimal spatial and temporal interpolation, which should be easier to work with for many applications. Gridded SOCAT is rich with information that has not been fully explored yet (e.g., regional differences in the seasonal cycles), but also contains biases and limitations that the user needs to recognize and address (e.g., local influences on values in some coastal regions).

A well-documented, publicly available, global data set of surface ocean carbon dioxide (CO2) parameters has been called for by international groups for nearly two decades. The Surface Ocean CO2 Atlas (SOCAT) project was initiated by the international marine carbon science community in 2007 with the aim of providing a comprehensive, publicly available, regularly updated, global data set of marine surface CO2, which had been subject to quality control (QC). Many additional CO2 data, not yet made public via the Carbon Dioxide Information Analysis Center (CDIAC), were retrieved from data originators, public websites and other data centres. All data were put in a uniform format following a strict protocol. Quality control was carried out according to clearly defined criteria. Regional specialists performed the quality control, using state-of-the-art web-based tools, specially developed for accomplishing this global team effort. SOCAT version 1.5 was made public in September 2011 and holds 6.3 million quality controlled surface CO2 data points from the global oceans and coastal seas, spanning four decades (1968–2007). Three types of data products are available: individual cruise files, a merged complete data set and gridded products. With the rapid expansion of marine CO2 data collection and the importance of quantifying net global oceanic CO2 uptake and its changes, sustained data synthesis and data access are priorities.

The globally integrated sea–air anthropogenic carbon dioxide (CO2) flux from 1990 to 2009 is determined from models and data-based approaches as part of the Regional Carbon Cycle Assessment and Processes (RECCAP) project. Numerical methods include ocean inverse models, atmospheric inverse models, and ocean general circulation models with parameterized biogeochemistry (OBGCMs). The median value of different approaches shows good agreement in average uptake. The best estimate of anthropogenic CO2 uptake for the time period based on a compilation of approaches is −2.0 Pg C yr−1. The interannual variability in the sea–air flux is largely driven by large-scale climate re-organizations and is estimated at 0.2 Pg C yr−1 for the two decades with some systematic differences between approaches. The largest differences between approaches are seen in the decadal trends. The trends range from −0.13 (Pg C yr−1) decade−1 to −0.50 (Pg C yr−1) decade−1 for the two decades under investigation. The OBGCMs and the data-based sea–air CO2 flux estimates show appreciably smaller decadal trends than estimates based on changes in carbon inventory suggesting that methods capable of resolving shorter timescales are showing a slowing of the rate of ocean CO2 uptake. RECCAP model outputs for five decades show similar differences in trends between approaches.

We examined potential interferences from water vapor and atmospheric background gases (N2, O2, and Ar), and biases by isotopologues of target species, on accurate measurement of atmospheric CO2 and CH4 by means of wavelength-scanned cavity ring-down spectroscopy (WS-CRDS). Changes of the background gas mole fractions in the sample air substantially impacted the CO2 and CH4 measurements: variation of CO2 and CH4 due to relative increase of each background gas increased as Ar < O2 < N2, suggesting similar relation for the pressure-broadening effects (PBEs) among the background gas. The pressure-broadening coefficients due to variations in O2 and Ar for CO2 and CH4 are empirically determined from these experimental results. Calculated PBEs using the pressure-broadening coefficients are linearly correlated with the differences between the mole fractions of O2 and Ar and their ambient abundances. Although the PBEs calculation showed that impact of natural variation of O2 is negligible on the CO2 and CH4 measurements, significant bias was inferred for the measurement of synthetic standard gases. For gas standards balanced with purified air, the PBEs were estimated to be marginal (up to 0.05 ppm for CO2 and 0.01 ppb for CH4) although the PBEs were substantial (up to 0.87 ppm for CO2 and 1.4 ppb for CH4) for standards balanced with synthetic air. For isotopic biases on CO2 measurements, we compared experimental results and theoretical calculations, which showed excellent agreement within their uncertainty. We derived instrument-specific water correction functions empirically for three WS-CRDS instruments (Picarro EnviroSense 3000i, G-1301, and G-2301), and evaluated the transferability of the water correction function from G-1301 among these instruments. Although the transferability was not proven, no significant difference was found in the water vapor correction function for the investigated WS-CRDS instruments as well as the instruments reported in the past studies within the typical analytical precision at sufficiently low water concentrations (2 and 4). For accurate measurements of CO2 and CH4 in ambient air, we concluded that WS-CRDS measurements should be performed under complete dehumidification of air samples, or moderate dehumidification followed by application of a water vapor correction function, along with calibration by natural air-based standard gases or purified air-balanced synthetic standard gases with the isotopic correction.

Some dominant spatial and temporal structures of the North Pacific air-sea CO2 fluxes in response to the Pacific Decadal Oscillation (PDO) are identified in three data products from three independent sources: an assimilated CO2 flux product and two forward model solutions. The interannual variability of CO2 flux is found to be an order of magnitude weaker compared to the seasonal cycle of CO2 flux in the North Pacific. A statistical approach is employed to quantify the signal-to-noise ratio in the reconstructed dataset to delineate the representativity errors. The dominant variability with a signal-to-noise ratio above one is identified and its correlations with PDO are examined. A tentative four-pole pattern in the North Pacific air-sea CO2 flux variability linked to PDO emerges in which two positively correlated poles are oriented in the northwest and southeast directions and contrarily, the negatively correlated poles are oriented in the northeast and southwest directions. This pattern is identified in three products, providing CO2 and pCO2. Its relations to the interannual El Niño-Southern Oscillation (ENSO) and lower-frequency PDO are separately identified. A combined EOF analysis between air-sea CO2 flux and key variables representing ocean-atmosphere interactions is carried out to elicit robust oscillations in the North Pacific CO2 flux in response to the PDO. The proposed spatial and temporal structures of the North Pacific CO2 fluxes are insightful since they separate the secular trends of the surface ocean carbon from the interannual variability. The regional characterization of the North Pacific in terms of PDO and CO2 flux variability is also instructive for determining the homogeneous oceanic domains for the Regional Carbon Cycle and Assessment Processes (RECCAP).

Long-term monitoring of carbon monoxide (CO) mixing ratios in the atmosphere over the Pacific Ocean is being carried out on commercial cargo vessels participating in the National Institute for Environmental Studies Voluntary Observing Ships program. The program provides a regular platform for measurement of atmospheric CO along four cruise routes: from Japan to Oceania, the United States, Canada, and Southeast Asia. Flask samples are collected during every cruise for subsequent analysis in the laboratory, and in 2005, continuous shipboard CO measurements were initiated on three of the routes. Here, we describe the system we developed for onboard measurement of CO mixing ratios with a commercially available gas filter correlation CO analyzer. The fully automated system measures CO in ambient air, and the detector sensitivity and background signals are calibrated by referencing the measurements to a CO-in-air standard gas (~1 ppmv) and to CO-free air scrubbed with a catalyst, respectively. We examined the artificial production of CO in the high-pressure working gas standards during storage by referencing the measurements to CO standard gases maintained as our primary scale before and after use on the ships. The onboard performance of the continuous CO measurement system was evaluated by comparing its data with data from laboratory analyses of flask samples using gas chromatography with a reduction gas detector. The reasonably good consistency between the two independent measurement methods demonstrated the good performance of both methods over the course of 3–5 years. The continuous measurement system was more useful than the flask sampling method for regionally polluted air masses, which were often encountered on Southeast Asian cruises.

Ocean acidification (decreases in carbonate ion concentration and pH) in response to rising atmospheric pCO2 is generally expected to reduce rates of calcification by reef calcifying organisms, with potentially severe implications for coral reef ecosystems. Large, algal symbiont-bearing benthic foraminifers, which are important primary and carbonate producers in coral reefs, produce high-Mg calcite shells, whose solubility can exceed that of aragonite produced by corals, making them the "first responder" in coral reefs to the decreasing carbonate saturation state of seawater. Here we report results of culture experiments performed to assess the effects of ongoing ocean acidification on the calcification of symbiont-bearing reef foraminifers using a high-precision pCO2 control system. Living clone individuals of three foraminiferal species (Baculogypsina sphaerulata, Calcarina gaudichaudii, and Amphisorus hemprichii) were subjected to seawater at five pCO2 levels from 260 to 970 μatm. Cultured individuals were maintained for about 12 weeks in an indoor flow-through system under constant water temperature, light intensity, and photoperiod. After the experiments, the shell diameter and weight of each cultured specimen were measured. Net calcification of B. sphaerulata and C. gaudichaudii, which secrete a hyaline shell and host diatom symbionts, increased under intermediate levels of pCO2 (580 and/or 770 μatm) and decreased at a higher pCO2 level (970 μatm). Net calcification of A. hemprichii, which secretes a porcelaneous shell and hosts dinoflagellate symbionts, tended to decrease at elevated pCO2. Observed different responses between hyaline and porcelaneous species are possibly caused by the relative importance of elevated pCO2, which induces CO2 fertilization effects by algal symbionts, versus associated changes in seawater carbonate chemistry, which decreases a carbonate concentration. Our findings suggest that ongoing ocean acidification might favor symbiont-bearing reef foraminifers with hyaline shells at intermediate pCO2 levels (580 to 770 μatm) but be unfavorable to those with either hyaline or porcelaneous shells at higher pCO2 levels (near 1000 μatm).