Global nitrous oxide production determined by oxygen sensitivity of nitrification and denitrification

The ocean is estimated to contribute up to ~20% of global fluxes of atmospheric nitrous oxide (N2O), an important greenhouse gas and ozone depletion agent. Marine oxygen minimum zones contribute disproportionately to this flux. To further understand the partition of nitrification and denitrification and their environmental controls on marine N2O fluxes, we report new relationships between oxygen concentration and rates of N2O production from nitrification and denitrification directly measured with 15N tracers in the Eastern Tropical Pacific. Highest N2O production rates occurred near the oxic‐anoxic interface, where there is strong potential for N2O efflux to the atmosphere. The dominant N2O source in oxygen minimum zones was nitrate reduction, the rates of which were 1 to 2 orders of magnitude higher than those of ammonium oxidation. The presence of oxygen significantly inhibited the production of N2O from both nitrification and denitrification. These experimental data provide new constraints to a multicomponent global ocean biogeochemical model, which yielded annual oceanic N2O efflux of 1.7–4.4 Tg‐N (median 2.8 Tg‐N, 1 Tg = 1012 g), with denitrification contributing 20% to the oceanic flux. Thus, denitrification should be viewed as a net N2O production pathway in the marine environment

Influence of Reduced Carbon Emissions and Oxidation on the Distribution of Atmospheric CO2: Implications for Inversion Analyses

Recent inverse analyses constraining carbon fluxes using atmospheric CO2 observations have assumed that the CO2 source from atmospheric oxidation of reduced carbon is released at the surface rather than distributed globally in the atmosphere. This produces a bias in the estimates of surface fluxes. We used a three-dimensional (3D) atmospheric chemistry model (GEOS-CHEM) to evaluate the magnitude of this effect on modeled concentrations and flux estimates. We find that resolving the 3D structure of the atmospheric CO2 source, as opposed to emitting this reduced carbon as CO2 at the surface, yields a decrease in the modeled annual mean interhemispheric gradient (N-S) of 0.21 ppm. Larger adjustments (up to −0.6 ppm) are apparent on a regional basis in and downwind of regions of high reduced carbon emissions. We used TransCom3 annual mean simulations from three transport models to evaluate the implications for inversion estimates. The main impacts are systematic decreases in estimates of northern continental land uptake (i.e., by 0.22 to 0.26 Pg C yr−1), and reductions in tropical land carbon efflux with smaller changes over oceans and in the Southern Hemisphere. These adjustments represent a systematic bias in flux estimates, accounting for changes of 9 to 27% in the estimated northern land CO2 sink for the three models evaluated here. Our results highlight the need for a realistic description of reduced carbon emission and oxidation processes in deriving inversion estimates of CO2 surface fluxes.Earth and Planetary SciencesEngineering and Applied Science

Influence of reduced carbon emissions and oxidation on the distribution of atmospheric CO_2: Implications for inversion analyses

Recent inverse analyses constraining carbon fluxes using atmospheric CO_2 observations have assumed that the CO_2 source from atmospheric oxidation of reduced carbon is released at the surface rather than distributed globally in the atmosphere. This produces a bias in the estimates of surface fluxes. We used a three‐dimensional (3D) atmospheric chemistry model (GEOS‐CHEM) to evaluate the magnitude of this effect on modeled concentrations and flux estimates. We find that resolving the 3D structure of the atmospheric CO_2 source, as opposed to emitting this reduced carbon as CO_2 at the surface, yields a decrease in the modeled annual mean interhemispheric gradient (N‐S) of 0.21 ppm. Larger adjustments (up to −0.6 ppm) are apparent on a regional basis in and downwind of regions of high reduced carbon emissions. We used TransCom3 annual mean simulations from three transport models to evaluate the implications for inversion estimates. The main impacts are systematic decreases in estimates of northern continental land uptake (i.e., by 0.22 to 0.26 Pg C yr^(−1)), and reductions in tropical land carbon efflux with smaller changes over oceans and in the Southern Hemisphere. These adjustments represent a systematic bias in flux estimates, accounting for changes of 9 to 27% in the estimated northern land CO_2 sink for the three models evaluated here. Our results highlight the need for a realistic description of reduced carbon emission and oxidation processes in deriving inversion estimates of CO_2 surface fluxes

Anthropogenic nitrogen inputs and impacts on oceanic N2O fluxes in the northern Indian Ocean: The need for an integrated observation and modelling approach

Anthropogenically-derived nitrogen input to the northern Indian Ocean has increased significantly in recent decades, based on both observational and model-derived estimates This external nutrient source is supplied by atmospheric deposition and riverine fluxes, and has the potential to affect the vulnerable biogeochemical systems of the Arabian Sea and Bay of Bengal, influencing productivity and oceanic production of the greenhouse-gas nitrous-oxide (N2O). We summarize current estimates of this external nitrogen source to the northern Indian Ocean from observations and models, highlight implications for regional marine N2O emissions using model-based analyses, and make recommendations for measurement and model needs to improve current estimates and future predictions of this impact. Current observationally-derived estimates of deposition and riverine nitrogen inputs are limited by sparse measurements and uncertainties on accurate characterization of nitrogen species composition. Ocean model assessments of the impact of external nitrogen sources on regional marine N2O production in the northern Indian Ocean estimate potentially significant changes but also have large associated uncertainties. We recommend an integrated program of basin-wide measurements combined with high-resolution modeling and more detailed characterization of nitrogen-cycle process to address these uncertainties and improve current estimates and predictions

Constraints on Asian and European sources of methane from CH 4 -C 2 H 6 -CO correlations in Asian outflow

Aircraft observations of Asian outflow from the Transport and Chemical Evolution Over the Pacific (TRACE-P) aircraft mission over the NW Pacific (March and April 2001) show large CH4 enhancements relative to background, as well as strong CH4-C2H6-CO correlations that provide signatures of regional sources. We apply a global chemical transport model simulation of the CH4-C2H6-CO system for the TRACE-P period to interpret these observations in terms of CH4 sources and to explore in particular the unique constraints from the CH4-C2H6-CO correlations. We use as a priori a global CH4 source inventory constrained with National Oceanic and Atmospheric Administration (NOAA) Climate Monitoring and Diagnostics Laboratory (CMDL) surface observations [Wang et al., 2004]. We find that the observed CH4 concentration enhancements and CH4-C2H6-CO correlations in Asian outflow in TRACE-P are determined mainly by anthropogenic emissions from China and Eurasia (defined here as Europe and eastern Russia), with only little contribution from tropical sources (wetlands and biomass burning). The a priori inventory overestimates the observed CH4 enhancements and shows regionally variable biases for the CH4/C2H6 slope. The CH4/CO slopes are simulated without significant bias. Matching both the observed CH4 enhancements and the CH4-C2H6-CO slopes in Asian outflow requires increasing the east Asian anthropogenic source of CH4, and decreasing the Eurasian anthropogenic source, by at least 30% for both. The need to increase the east Asian source is driven by the underestimate of the CH4/C2H6 slope in boundary layer Chinese outflow. The Streets et al. [2003] anthropogenic emission inventory for east Asia fits this constraint by increasing CH4 emissions from that region by 40% relative to the a priori, largely because of higher livestock and landfill source estimates. Eurasian sources (mostly European) then need to be reduced by 30–50% from the a priori value of 68 Tg yr−1. The decrease of European sources could result in part from recent mitigation of emissions from coal mining and landfills.Engineering and Applied Science

Evaluation of ocean dimethylsulfide concentration and emission in CMIP6 models

Characteristics and trends of surface ocean dimethylsulfide (DMS) concentrations and fluxes into the atmosphere of four Earth system models (ESMs: CNRM-ESM2-1, MIROC-ES2L, NorESM2-LM, and UKESM1-0-LL) are analysed over the recent past (1980–2009) and into the future, using Coupled Model Intercomparison Project 6 (CMIP6) simulations. The DMS concentrations in historical simulations systematically underestimate the most widely used observed climatology but compare more favourably against two recent observation-based datasets. The models better reproduce observations in mid to high latitudes, as well as in polar and westerlies marine biomes. The resulting multi-model estimate of contemporary global ocean DMS emissions is 16–24 Tg S yr−1, which is narrower than the observational-derived range of 16 to 28 Tg S yr−1. The four models disagree on the sign of the trend of the global DMS flux from 1980 onwards, with two models showing an increase and two models a decrease. At the global scale, these trends are dominated by changes in surface DMS concentrations in all models, irrespective of the air–sea flux parameterisation used. In turn, three models consistently show that changes in DMS concentrations are correlated with changes in marine productivity; however, marine productivity is poorly constrained in the current generation of ESMs, thus limiting the predictive ability of this relationship. In contrast, a consensus is found among all models over polar latitudes where an increasing trend is predominantly driven by the retreating sea-ice extent. However, the magnitude of this trend between models differs by a factor of 3, from 2.9 to 9.2 Gg S decade−1 over the period 1980–2014, which is at the low end of a recent satellite-derived analysis. Similar increasing trends are found in climate projections over the 21st century

The impacts of ocean acidification on marine trace gases and the implications for atmospheric chemistry and climate

Surface ocean biogeochemistry and photochemistry regulate ocean–atmosphere fluxes of trace gases critical for Earth’s atmospheric chemistry and climate. The oceanic processes governing these fluxes are often sensitive to the changes in ocean pH (or pCO2) accompanying ocean acidification (OA), with potential for future climate feedbacks. Here, we review current understanding (from observational, experimental and model studies) on the impact of OA on marine sources of key climate-active trace gases, including dimethyl sulfide (DMS), nitrous oxide (N2O), ammonia and halocarbons. We focus on DMS, for which available information is considerably greater than for other trace gases. We highlight OA-sensitive regions such as polar oceans and upwelling systems, and discuss the combined effect of multiple climate stressors (ocean warming and deoxygenation) on trace gas fluxes. To unravel the biological mechanisms responsible for trace gas production, and to detect adaptation, we propose combining process rate measurements of trace gases with longer term experiments using both model organisms in the laboratory and natural planktonic communities in the field. Future ocean observations of trace gases should be routinely accompanied by measurements of two components of the carbonate system to improve our understanding of how in situ carbonate chemistry influences trace gas production. Together, this will lead to improvements in current process model capabilities and more reliable predictions of future global marine trace gas fluxes

Inverse modeling of CO2 sources and sinks using satellite observations of CO2 from TES and surface flask measurements

We infer CO2 surface fluxes using satellite observations of mid-tropospheric CO2 from the Tropospheric Emission Spectrometer (TES) and measurements of CO2 from surface flasks in a time-independent inversion analysis based on the GEOS-Chem model. Using TES CO2 observations over oceans, spanning 40° S–40° N, we find that the horizontal and vertical coverage of the TES and flask data are complementary. This complementarity is demonstrated by combining the datasets in a joint inversion, which provides better constraints than from either dataset alone, when a posteriori CO2 distributions are evaluated against independent ship and aircraft CO2 data. In particular, the joint inversion offers improved constraints in the tropics where surface measurements are sparse, such as the tropical forests of South America. Aggregating the annual surface-to-atmosphere fluxes from the joint inversion for the year 2006 yields −1.13±0.21 Pg C for the global ocean, −2.77±0.20 Pg C for the global land biosphere and −3.90±0.29 Pg C for the total global natural flux (defined as the sum of all biospheric, oceanic, and biomass burning contributions but excluding CO2 emissions from fossil fuel combustion). These global ocean and global land fluxes are shown to be near the median of the broad range of values from other inversion results for 2006. To achieve these results, a bias in TES CO2 in the Southern Hemisphere was assessed and corrected using aircraft flask data, and we demonstrate that our results have low sensitivity to variations in the bias correction approach. Overall, this analysis suggests that future carbon data assimilation systems can benefit by integrating in situ and satellite observations of CO2 and that the vertical information provided by satellite observations of mid-tropospheric CO2 combined with measurements of surface CO2, provides an important additional constraint for flux inversions

A surface ocean CO2 reference network, SOCONET and associated marine boundary layer CO2 measurements

The Surface Ocean CO2 NETwork (SOCONET) and atmospheric Marine Boundary Layer (MBL) CO2 measurements from ships and buoys focus on the operational aspects of measurements of CO2 in both the ocean surface and atmospheric MBLs. The goal is to provide accurate pCO2 data to within 2 micro atmosphere (μatm) for surface ocean and 0.2 parts per million (ppm) for MBL measurements following rigorous best practices, calibration and intercomparison procedures. Platforms and data will be tracked in near real-time and final quality-controlled data will be provided to the community within a year. The network, involving partners worldwide, will aid in production of important products such as maps of monthly resolved surface ocean CO2 and air-sea CO2 flux measurements. These products and other derivatives using surface ocean and MBL CO2 data, such as surface ocean pH maps and MBL CO2 maps, will be of high value for policy assessments and socio-economic decisions regarding the role of the ocean in sequestering anthropogenic CO2 and how this uptake is impacting ocean health by ocean acidification. SOCONET has an open ocean emphasis but will work with regional (coastal) networks. It will liaise with intergovernmental science organizations such as Global Atmosphere Watch (GAW), and the joint committee for and ocean and marine meteorology (JCOMM). Here we describe the details of this emerging network and its proposed operations and practices