A large source of atmospheric nitrous oxide from subtropical North Pacific surface waters

Nitrous oxide (N2O), a trace gas whose concentration is increasing in the atmosphere, plays an important role in both radiative forcing and stratospheric ozone depletion,. Its biogeochemical cycle has thus come under intense scrutiny in recent years. Despite these efforts, the global budget of N2O remains unresolved, and the nature and magnitude of the sources and sinks continue to be debated despite the constraints that can be provided by characterizations of the gas,. We report here the results of dual-isotope measurements of N2O from the water column of the subtropical North Pacific Ocean. Nitrous oxide within the lower-euphotic and upper-aphotic zones is depleted in both 15N and 18O relative to its tropospheric and deep-ocean composition. These findings are consistent with a prediction, based on global mass-balance considerations, of a near-surface isotopically depleted oceanic N2O source. Our results indicate that this source, probably produced by bacterial nitrification, contributes significantly to the ocean–atmosphere flux of N2O in the oligotrophic subtropical North Pacific Ocean. This source may act to buffer the isotopic composition of tropospheric N2O, and is quantitatively significant in the global tropospheric N2O budget. Because dissolved gases in near-surface waters are more readily exchanged with the atmospheric reservoir than those in deep waters, the existence of a quantitatively significant N2O source at a relatively shallow depth has potentially important implications for the susceptibility of the source, and the ocean–atmosphere flux, to climatic influences.

[1]  A. Alldredge,et al.  Can Microscale Chemical Patches Persist in the Sea? Microelectrode Study of Marine Snow, Fecal Pellets , 1987, Science.

[2]  B. Jørgensen A theoretical model of the stable sulfur isotope distribution in marine sediments , 1979 .

[3]  T. Saino,et al.  15N/14N ratio of dissolved N2O in the eastern tropical Pacific Ocean , 1984, Nature.

[4]  J. Houghton,et al.  Climate change : the IPCC scientific assessment , 1990 .

[5]  D. Karl,et al.  Nitrification in the euphotic zone as a source for nitrite, nitrate, and nitrous oxide at Station ALOHA , 1996 .

[6]  A. Bouwman,et al.  Uncertainties in the global source distribution of nitrous oxide , 1995 .

[7]  W. Brand PreCon: A Fully Automated Interface for the Pre-Gc Concentration of Trace Gases on Air for Isotopic Analysis , 1995 .

[8]  H. Craig Isotopic standards for carbon and oxygen and correction factors for mass-spectrometric analysis of carbon dioxide , 1957 .

[9]  S. Naqvi,et al.  Nitrous oxide in the Arabian Sea , 1991 .

[10]  B. Popp,et al.  Stable Carbon Isotopic Analysis of Low-Level Methane in Water and Gas , 1997 .

[11]  N. Yoshida,et al.  Nitrogen isotope ratio of atmospheric N2O as a key to the global cycle of N2O , 1983 .

[12]  R. Weiss,et al.  Global oceanic emissions of nitrous oxide , 1995 .

[13]  B. Popp,et al.  Determination of Concentration and Carbon Isotopic Composition of Dissolved Methane in Sediments and Nearshore Waters , 1995 .

[14]  C. Law,et al.  Significant flux of atmospheric nitrous oxide from the northwest Indian Ocean , 1990, Nature.

[15]  Michael B. McElroy,et al.  Evidence for an additional source of atmospheric N2O , 1996 .

[16]  T. Yoshinari,et al.  Oxygen isotope ratios in N2O from nitrification at a wastewater treatment facility , 1985, Nature.

[17]  W. Broecker,et al.  The average vertical mixing coefficient for the oceanic thermocline , 1984 .

[18]  N. Yoshida,et al.  N2O Reduction by Azotobacter vinelandii with Emphasis on Kinetic Nitrogen Isotope Effects , 1987 .

[19]  L. Codispoti,et al.  Nitrification, denitrification and nitrous oxide cycling in the eastern tropical South Pacific ocean , 1985 .

[20]  H. Craig,et al.  Two-isotope characterization of N20 in the Pacific Ocean and constraints on its origin in deep water , 1990, Nature.

[21]  Ricardo M Letelier,et al.  Ecosystem changes in the North Pacific subtropical gyre attributed to the 1991–92 El Niño , 1995, Nature.

[22]  N. Yoshida 15N-depleted N2O as a product of nitrification , 1988, Nature.

[23]  Rahn,et al.  Stable isotope enrichment in stratospheric nitrous oxide , 1997, Science.

[24]  David M. Karl,et al.  The Hawaii Ocean Time-series (HOT) program: Background, rationale and field implementation , 1996 .

[25]  P. Crutzen The influence of nitrogen oxides on the atmospheric ozone content , 1970 .

[26]  D. Wisegarver,et al.  Nitrous oxide and vertical mixing in the equatorial Pacific during the 1982–1983 El Niño , 1987 .

[27]  H. Craig,et al.  Nitrogen-15 and Oxygen-18 Characteristics of Nitrous Oxide: A Global Perspective , 1993, Science.

[28]  L. Codispoti,et al.  Budgetary and biogeochemical implications of N2O isotope signatures in the Arabian Sea , 1998, Nature.

[29]  L. Codispoti,et al.  Nitrogen and oxygen isotopic composition of N2O from suboxic waters of the eastern tropical North Pacific and the Arabian Sea—measurement by continuous-flow isotope-ratio monitoring , 1997 .