Atmos. Chem. Phys. Discuss., 13, 19471-19525, 2013
www.atmos-chem-phys-discuss.net/13/19471/2013/
doi:10.5194/acpd-13-19471-2013
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under the Creative Commons Attribution 3.0 License.
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Global and regional emissions estimates for N2O
E. Saikawa1,2, R. G. Prinn1, E. Dlugokencky3, K. Ishijima4, G. S. Dutton3,5, B. D. Hall3, R. Langenfelds6, Y. Tohjima7, T. Machida7, M. Manizza8, M. Rigby9, S. O'Doherty9, P. K. Patra4, C. M. Harth8, R. F. Weiss8, P. B. Krummel6, M. van der Schoot6, P. B. Fraser6, L. P. Steele6, S. Aoki10, T. Nakazawa10, and J. W. Elkins3
1Center for Global Change Science, Massachusetts Institute of Technology, Cambridge, MA, USA
2Department of Environmental Studies, Emory University, Atlanta, GA, USA
3Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
4Research Institute for Global Change, Japan Agency for Marine-Earth Science and Technology, Yokohama, Japan
5Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
6Centre for Australian Weather and Climate Research, CSIRO Marine and Atmospheric Research, Aspendale, Victoria, Australia
7National Institute for Environmental Studies, Tsukuba, Japan
8Scripps Institution of Oceanography, University of California, San Diego, La Jolla, California, USA
9School of Chemistry, University of Bristol, Bristol, UK
10Center for Atmospheric and Oceanic Studies, Tohoku University, Sendai, Japan

Abstract. We present a comprehensive estimate of nitrous oxide ( N2O) emissions using observations and models from 1995 to 2008. High-frequency records of tropospheric N2O are available from measurements at Cape Grim, Tasmania; Cape Matatula, American Samoa; Ragged Point, Barbados; Mace Head, Ireland; and at Trinidad Head, California using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. The Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also discrete air samples collected in flasks and in situ measurements from remote sites across the globe and analyzed them for a suite of species including N2O. In addition to these major networks, we include in situ and aircraft measurements from the National Institute for Environmental Studies (NIES) and flask measurements from the Tohoku University and Commonwealth Scientific and Industrial Research Organization (CSIRO) networks. All measurements show increasing atmospheric mole fractions of N2O, with a varying growth rate of 0.1–0.7 % yr-1, resulting in a 7.4% increase in the background atmospheric mole fraction between 1979 and 2011. Using existing emission inventories as well as bottom-up process modeling results, we first create globally-gridded a priori N2O emissions over the 37 yr since 1975. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4), and a Bayesian inverse method to estimate global as well as regional annual emissions for five source sectors from 13 regions in the world. This is the first time that all of these measurements from multiple networks have been combined to determine emissions. Our inversion indicates that global and regional N2O emissions have an increasing trend between 1995 and 2008. Despite large uncertainties, a significant increase is seen from the Asian agricultural sector in the recent years, most likely due to an increase in the use of nitrogenous fertilizers, as has been suggested by previous studies, and also in Asian natural soil.

Citation: Saikawa, E., Prinn, R. G., Dlugokencky, E., Ishijima, K., Dutton, G. S., Hall, B. D., Langenfelds, R., Tohjima, Y., Machida, T., Manizza, M., Rigby, M., O'Doherty, S., Patra, P. K., Harth, C. M., Weiss, R. F., Krummel, P. B., van der Schoot, M., Fraser, P. B., Steele, L. P., Aoki, S., Nakazawa, T., and Elkins, J. W.: Global and regional emissions estimates for N2O, Atmos. Chem. Phys. Discuss., 13, 19471-19525, doi:10.5194/acpd-13-19471-2013, 2013.
 
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