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The air–sea exchange and oceanic cycling of greenhouse gases (GHG), including carbon dioxide (CO2), nitrous oxide (N2O), methane (CH4), carbon monoxide (CO), and nitrogen oxides (NOx = NO + NO2), are fundamental in controlling the evolution of the Earth’s atmospheric chemistry and climate. Significant advances have been made over the last 10 years in understanding, instrumentation and methods, as well as deciphering the production and consumption pathways of GHG in the upper ocean (including the surface and subsurface ocean down to approximately 1000 m). The global ocean under current conditions is now well established as a major sink for CO2, a major source for N2O and a minor source for both CH4 and CO. The importance of the ocean as a sink or source of NOx is largely unknown so far. There are still considerable uncertainties about the processes and their major drivers controlling the distributions of N2O, CH4, CO, and NOx in the upper ocean. Without having a fundamental understanding of oceanic GHG production and consumption pathways, our knowledge about the effects of ongoing major oceanic changes—warming, acidification, deoxygenation, and eutrophication—on the oceanic cycling and air–sea exchange of GHG remains rudimentary at best. We suggest that only through a comprehensive, coordinated, and interdisciplinary approach that includes data collection by global observation networks as well as joint process studies can the necessary data be generated to (1) identify the relevant microbial and phytoplankton communities, (2) quantify the rates of ocean GHG production and consumption pathways, (3) comprehend their major drivers, and (4) decipher economic and cultural implications of mitigation solutions.more » « less
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Abstract. Nitrous oxide (N2O) is a long-lived potent greenhouse gas and stratospheric ozone-depleting substance that has been accumulating in the atmosphere since the preindustrial period. The mole fraction of atmospheric N2O has increased by nearly 25 % from 270 ppb (parts per billion) in 1750 to 336 ppb in 2022, with the fastest annual growth rate since 1980 of more than 1.3 ppb yr−1 in both 2020 and 2021. According to the Sixth Assessment Report of the Intergovernmental Panel on Climate Change (IPCC AR6), the relative contribution of N2O to the total enhanced effective radiative forcing of greenhouse gases was 6.4 % for 1750–2022. As a core component of our global greenhouse gas assessments coordinated by the Global Carbon Project (GCP), our global N2O budget incorporates both natural and anthropogenic sources and sinks and accounts for the interactions between nitrogen additions and the biogeochemical processes that control N2O emissions. We use bottom-up (BU: inventory, statistical extrapolation of flux measurements, and process-based land and ocean modeling) and top-down (TD: atmospheric measurement-based inversion) approaches. We provide a comprehensive quantification of global N2O sources and sinks in 21 natural and anthropogenic categories in 18 regions between 1980 and 2020. We estimate that total annual anthropogenic N2O emissions have increased 40 % (or 1.9 Tg N yr−1) in the past 4 decades (1980–2020). Direct agricultural emissions in 2020 (3.9 Tg N yr−1, best estimate) represent the large majority of anthropogenic emissions, followed by other direct anthropogenic sources, including fossil fuel and industry, waste and wastewater, and biomass burning (2.1 Tg N yr−1), and indirect anthropogenic sources (1.3 Tg N yr−1) . For the year 2020, our best estimate of total BU emissions for natural and anthropogenic sources was 18.5 (lower–upper bounds: 10.6–27.0) Tg N yr−1, close to our TD estimate of 17.0 (16.6–17.4) Tg N yr−1. For the 2010–2019 period, the annual BU decadal-average emissions for both natural and anthropogenic sources were 18.2 (10.6–25.9) Tg N yr−1 and TD emissions were 17.4 (15.8–19.20) Tg N yr−1. The once top emitter Europe has reduced its emissions by 31 % since the 1980s, while those of emerging economies have grown, making China the top emitter since the 2010s. The observed atmospheric N2O concentrations in recent years have exceeded projected levels under all scenarios in the Coupled Model Intercomparison Project Phase 6 (CMIP6), underscoring the importance of reducing anthropogenic N2O emissions. To evaluate mitigation efforts and contribute to the Global Stocktake of the United Nations Framework Convention on Climate Change, we propose the establishment of a global network for monitoring and modeling N2O from the surface through to the stratosphere. The data presented in this work can be downloaded from https://doi.org/10.18160/RQ8P-2Z4R (Tian et al., 2023).more » « less
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Abstract. Oxygen-deficient zones (ODZs) are major sites of net naturalnitrous oxide (N2O) production and emissions. In order to understandchanges in the magnitude of N2O production in response to globalchange, knowledge on the individual contributions of the major microbialpathways (nitrification and denitrification) to N2O production andtheir regulation is needed. In the ODZ in the coastal area off Peru, thesensitivity of N2O production to oxygen and organic matter wasinvestigated using 15N tracer experiments in combination with quantitative PCR (qPCR) andmicroarray analysis of total and active functional genes targeting archaeal amoAand nirS as marker genes for nitrification and denitrification, respectively.Denitrification was responsible for the highest N2O production with amean of 8.7 nmol L−1 d−1 but up to 118±27.8 nmol L−1 d−1 just below the oxic–anoxic interface. The highest N2O productionfrom ammonium oxidation (AO) of 0.16±0.003 nmol L−1 d−1occurred in the upper oxycline at O2 concentrations of 10–30 µmol L−1 which coincided with the highest archaeal amoA transcripts/genes.Hybrid N2O formation (i.e., N2O with one N atom from NH4+and the other from other substrates such as NO2-) was the dominantspecies, comprising 70 %–85 % of total produced N2O fromNH4+, regardless of the ammonium oxidation rate or O2concentrations. Oxygen responses of N2O production varied withsubstrate, but production and yields were generally highest below 10 µmol L−1 O2. Particulate organic matter additions increasedN2O production by denitrification up to 5-fold, suggesting increasedN2O production during times of high particulate organic matter export.High N2O yields of 2.1 % from AO were measured, but the overallcontribution by AO to N2O production was still an order of magnitudelower than that of denitrification. Hence, these findings show thatdenitrification is the most important N2O production process in low-oxygen conditions fueled by organic carbon supply, which implies a positivefeedback of the total oceanic N2O sources in response to increasingoceanic deoxygenation.more » « less
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null (Ed.)Abstract. In the current era of rapid climate change, accuratecharacterization of climate-relevant gas dynamics – namely production,consumption, and net emissions – is required for all biomes, especially thoseecosystems most susceptible to the impact of change. Marine environmentsinclude regions that act as net sources or sinks for numerous climate-activetrace gases including methane (CH4) and nitrous oxide (N2O). Thetemporal and spatial distributions of CH4 and N2O are controlledby the interaction of complex biogeochemical and physical processes. Toevaluate and quantify how these mechanisms affect marine CH4 andN2O cycling requires a combination of traditional scientificdisciplines including oceanography, microbiology, and numerical modeling.Fundamental to these efforts is ensuring that the datasets produced byindependent scientists are comparable and interoperable. Equally critical istransparent communication within the research community about the technicalimprovements required to increase our collective understanding of marineCH4 and N2O. A workshop sponsored by Ocean Carbon and Biogeochemistry (OCB)was organized to enhance dialogue and collaborations pertaining tomarine CH4 and N2O. Here, we summarize the outcomes from theworkshop to describe the challenges and opportunities for near-futureCH4 and N2O research in the marine environment.more » « less
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Abstract. Large-scale climatic forcing is impactingoceanic biogeochemical cycles and is expected to influence the water-columndistribution of trace gases, including methane and nitrous oxide. Our abilityas a scientific community to evaluate changes in the water-column inventoriesof methane and nitrous oxide depends largely on our capacity to obtain robustand accurate concentration measurements that can be validated acrossdifferent laboratory groups. This study represents the first formalinternational intercomparison of oceanic methane and nitrous oxidemeasurements whereby participating laboratories received batches of seawatersamples from the subtropical Pacific Ocean and the Baltic Sea. Additionally,compressed gas standards from the same calibration scale were distributed tothe majority of participating laboratories to improve the analytical accuracyof the gas measurements. The computations used by each laboratory to derivethe dissolved gas concentrations were also evaluated for inconsistencies(e.g., pressure and temperature corrections, solubility constants). Theresults from the intercomparison and intercalibration provided invaluableinsights into methane and nitrous oxide measurements. It was observed thatanalyses of seawater samples with the lowest concentrations of methane andnitrous oxide had the lowest precisions. In comparison, while the analyticalprecision for samples with the highest concentrations of trace gases wasbetter, the variability between the different laboratories was higher:36% for methane and 27% for nitrous oxide. In addition, thecomparison of different batches of seawater samples with methane and nitrousoxide concentrations that ranged over an order of magnitude revealed theramifications of different calibration procedures for each trace gas.Finally, this study builds upon the intercomparison results to developrecommendations for improving oceanic methane and nitrous oxide measurements,with the aim of precluding future analytical discrepancies betweenlaboratories.more » « less
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