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Thompson, RL, Chevallier F, Crotwell AM, Dutton G, Langenfelds RL, Prinn RG, Weiss RF, Tohjima Y, Nakazawa T, Krummel PB, Steele LP, Fraser P, O'Doherty S, Ishijima K, Aoki S.  2014.  Nitrous oxide emissions 1999 to 2009 from a global atmospheric inversion. Atmospheric Chemistry and Physics. 14:1801-1817.   10.5194/acp-14-1801-2014   AbstractWebsite

N2O surface fluxes were estimated for 1999 to 2009 using a time-dependent Bayesian inversion technique. Observations were drawn from 5 different networks, incorporating 59 surface sites and a number of ship-based measurement series. To avoid biases in the inverted fluxes, the data were adjusted to a common scale and scale offsets were included in the optimization problem. The fluxes were calculated at the same resolution as the transport model (3.75 degrees longitude x 2.5 degrees latitude) and at monthly time resolution. Over the 11-year period, the global total N2O source varied from 17.5 to 20.1 Tg a(-1) N. Tropical and subtropical land regions were found to consistently have the highest N2O emissions, in particular in South Asia (20 +/- 3% of global total), South America (13 +/- 4 %) and Africa (19 +/- 3 %), while emissions from temperate regions were smaller: Europe (6 +/- 1 %) and North America (7 +/- 2 %). A significant multi-annual trend in N2O emissions (0.045 Tg a(-2) N) from South Asia was found and confirms inventory estimates of this trend. Considerable interannual variability in the global N2O source was observed (0.8 Tg a(-1) N, 1 standard deviation, SD) and was largely driven by variability in tropical and subtropical soil fluxes, in particular in South America (0.3 Tg a(-1) N, 1 SD) and Africa (0.3 Tg a(-1) N, 1 SD). Notable variability was also found for N2O fluxes in the tropical and southern oceans (0.15 and 0.2 Tg a(-1) N, 1 SD, respectively). Interannual variability in the N2O source shows some correlation with the El Nino-Southern Oscillation (ENSO), where El Nino conditions are associated with lower N2O fluxes from soils and from the ocean and vice versa for La Nina conditions.

Thompson, RL, Dlugokencky E, Chevallier F, Ciais P, Dutton G, Elkins JW, Langenfelds RL, Prinn RG, Weiss RF, Tohjima Y, O'Doherty S, Krummel PB, Fraser P, Steele LP.  2013.  Interannual variability in tropospheric nitrous oxide. Geophysical Research Letters. 40:4426-4431.   10.1002/grl.50721   AbstractWebsite

Observations of tropospheric N2O mixing ratio show significant variability on interannual timescales (0.2ppb, 1 standard deviation). We found that interannual variability in N2O is weakly correlated with that in CFC-12 and SF6 for the northern extratropics and more strongly correlated for the southern extratropics, suggesting that interannual variability in all these species is influenced by large-scale atmospheric circulation changes and, for SF6 in particular, interhemispheric transport. N2O interannual variability was not, however, correlated with polar lower stratospheric temperature, which is used as a proxy for stratosphere-to-troposphere transport in the extratropics. This suggests that stratosphere-to-troposphere transport is not a dominant factor in year-to-year variations in N2O growth rate. Instead, we found strong correlations of N2O interannual variability with the Multivariate ENSO Index. The climate variables, precipitation, soil moisture, and temperature were also found to be significantly correlated with N2O interannual variability, suggesting that climate-driven changes in soil N2O flux may be important for variations in N2O growth rate.

Simmonds, PG, Manning AJ, Athanassiadou M, Scaife AA, Derwent RG, O'Doherty S, Harth CM, Weiss RF, Dutton GS, Hall BD, Sweeney C, Elkins JW.  2013.  Interannual fluctuations in the seasonal cycle of nitrous oxide and chlorofluorocarbons due to the Brewer-Dobson circulation. Journal of Geophysical Research-Atmospheres. 118:10694-10706.   10.1002/jgrd.50832   AbstractWebsite

The tropospheric seasonal cycles of N2O, CFC-11 (CCl3F), and CFC-12 (CCl2F2) are influenced by atmospheric dynamics. The interannually varying summertime minima in mole fractions of these trace gases have been attributed to interannual variations in mixing of stratospheric air (depleted in CFCs and N2O) with tropospheric air with a few months lag. The amount of wave activity that drives the stratospheric circulation and influences the winter stratospheric jet and subsequent mass transport across the tropopause appears to be the primary cause of this interannual variability. We relate the observed seasonal minima of species at three Northern Hemisphere sites (Mace Head, Ireland; Trinidad Head, U.S.; and Barrow, Alaska) with the behavior of the winter stratospheric jet. As a result, a good correlation is obtained between zonal winds in winter at 10 hPa, 58°N–68°N, and the detrended seasonal minima in the stratosphere-influenced tracers. For these three tracers, individual Pearson correlation coefficients (r) between 0.51 and 0.71 were found, with overall correlations of between 0.67 and 0.77 when “composite species” were considered. Finally, we note that the long-term observations of CFCs and N2O in the troposphere provide an independent monitoring method complementary to satellite data. Furthermore, they could provide a useful observational measure of the strength of stratosphere-troposphere exchange and, thus, could be used to monitor any long-term trend in the Brewer-Dobson circulation which is predicted by climate models to increase over the coming decades.

Nevison, CD, Dlugokencky E, Dutton G, Elkins JW, Fraser P, Hall B, Krummel PB, Langenfelds RL, O'Doherty S, Prinn RG, Steele LP, Weiss RF.  2011.  Exploring causes of interannual variability in the seasonal cycles of tropospheric nitrous oxide. Atmospheric Chemistry and Physics. 11:3713-3730.   10.5194/acp-11-3713-2011   AbstractWebsite

Seasonal cycles in the mixing ratios of tropospheric nitrous oxide (N(2)O) are derived by detrending long-term measurements made at sites across four global surface monitoring networks. The detrended monthly data display large interannual variability, which at some sites challenges the concept of a "mean" seasonal cycle. In the Northern Hemisphere, correlations between polar winter lower stratospheric temperature and detrended N(2)O data, around the month of the seasonal minimum, provide empirical evidence for a stratospheric influence, which varies in strength from year to year and can explain much of the interannual variability in the surface seasonal cycle. Even at sites where a strong, competing, regional N(2)O source exists, such as from coastal upwelling at Trinidad Head, California, the stratospheric influence must be understood to interpret the biogeochemical signal in monthly mean data. In the Southern Hemisphere, detrended surface N(2)O monthly means are correlated with polar spring lower stratospheric temperature in months preceding the N(2)O minimum, providing empirical evidence for a coherent stratospheric influence in that hemisphere as well, in contrast to some recent atmospheric chemical transport model (ACTM) results. Correlations between the phasing of the surface N(2)O seasonal cycle in both hemispheres and both polar lower stratospheric temperature and polar vortex break-up date provide additional support for a stratospheric influence. The correlations discussed above are generally more evident in high-frequency in situ data than in data from weekly flask samples. Furthermore, the interannual variability in the N(2)O seasonal cycle is not always correlated among in situ and flask networks that share common sites, nor do the mean seasonal amplitudes always agree. The importance of abiotic influences such as the stratospheric influx and tropospheric transport on N(2)O seasonal cycles suggests that, at sites remote from local sources, surface N(2)O mixing ratio data by themselves are unlikely to provide information about seasonality in surface sources, e. g., for atmospheric inversions, unless the ACTMs employed in the inversions accurately account for these influences. An additional abioitc influence is the seasonal ingassing and outgassing of cooling and warming surface waters, which creates a thermal signal in tropospheric N(2)O that is of particular importance in the extratropical Southern Hemisphere, where it competes with the biological ocean source signal.

Huang, J, Golombek A, Prinn R, Weiss R, Fraser P, Simmonds P, Dlugokencky EJ, Hall B, Elkins J, Steele P, Langenfelds R, Krummel P, Dutton G, Porter L.  2008.  Estimation of regional emissions of nitrous oxide from 1997 to 2005 using multinetwork measurements, a chemical transport model, and an inverse method. Journal of Geophysical Research-Atmospheres. 113   10.1029/2007jd009381   AbstractWebsite

Nitrous oxide (N2O) is an important ozone-depleting gas and greenhouse gas with multiple uncertain emission processes. Global nitrous oxide observations, the Model of Atmospheric Transport and Chemistry (MATCH) and an inverse method were used to optimally estimate N2O emissions from twelve source regions around the globe. MATCH was used with forecast center reanalysis winds at T62 resolution (192 longitude by 94 latitude surface grid, and 28 vertical levels) from 1 July 1996 to 30 June 2006. The average concentrations of N2O in the lowest four layers of the model were then compared with the monthly mean observations from four national/international networks measuring at 65 surface sites. A 12-month-running-mean smoother was applied to both the model results and the observations, due to the fact that the model was not able to reproduce the very small observed seasonal cycles. The inverse method was then used to solve for the time-averaged regional emissions of N2O for two time periods (1 January 1997 to 31 December 2001 and 1 January 2002 to 31 December 2005). The best estimate inversions assume that the model stratospheric destruction rates, which lead to a global N2O lifetime of 125 years, are correct. It also assumes normalized emission spatial distributions within each region from Bouwman et al. (1995). We conclude that global N2O emissions with 66% probability errors are 16.3(-1.2)(+1.5) and 15.4(-1.3)(+1.7) TgN (N2O) a(-1), for 1997-2001 and 2001-2005 respectively. Emissions from the equator to 30 degrees N increased significantly from the initial Bouwman et al. (1995) estimates while emissions from southern oceans (30 degrees S-90 degrees S) decreased significantly. The quoted uncertainties include both the measurement errors and modeling uncertainties estimated using a separate flexible 12-box model. We also found that 23 +/- 4% of the N2O global total emissions come from the ocean, which is slightly smaller than the Bouwman et al. (1995) estimate. For the estimation of emissions from the twelve model regions, we conclude that, relative to Bouwman et al. (1995), land emissions from South America, Africa, and China/Japan/South East Asia are larger, while land emissions from Australia/New Zealand are smaller. Our study also shows a shift of the oceanic sources from the extratropical to the tropical oceans relative to Bouwman et al. (1995). Between the periods 1997-2001 and 2002-2005, emissions increased in China/Japan/South East Asia, 0 degrees-30 degrees N oceans, and North West Asia and decreased in Australia/New Zealand, 30 degrees S-90 degrees S oceans, 30 degrees N-90 degrees N oceans, and Africa. The lower tropical ocean emissions in 1997-2001 relative to 2002-2005 could result from the effects of the 1997-1998 El Nino in the earlier period.

Nevison, CD, Kinnison DE, Weiss RF.  2004.  Stratospheric influences on the tropospheric seasonal cycles of nitrous oxide and chlorofluorocarbons. Geophysical Research Letters. 31   10.1029/2004gl020398   AbstractWebsite

The stratospheric influence on the tropospheric seasonal cycles of N2O, CFC-11 ( CCl3F), CFC-12 (CCl2F2) and CFC-113 (CCl2FCClF2) is investigated using observations from the AGAGE global trace gas monitoring network and the results of the Whole Atmosphere Community Climate Model (WACCM). WACCM provides the basis for a number of predictions about the relative amplitudes of N2O and CFC seasonal cycles and about the relative magnitude and phasing of seasonal cycles in the northern and southern hemispheres. These predictions are generally consistent with observations, suggesting that the stratosphere exerts a coherent influence on the tropospheric seasonal cycles of trace gases whose primary sinks are in the stratosphere. This stratospheric influence may complicate efforts to validate estimated source distributions of N2O, an important greenhouse gas, in atmospheric transport model studies.

Nevison, CD, Weiss RF, Erickson DJ.  1995.  Global oceanic emissions of nitrous oxide. Journal of Geophysical Research-Oceans. 100:15809-15820.   10.1029/95jc00684   AbstractWebsite

The global N2O flux from the ocean to the atmosphere is calculated based on more than 60,000 expedition measurements of the N2O anomaly in surface water. The expedition data are extrapolated globally and coupled to daily air-sea gas transfer coefficients modeled at 2.8 degrees x 2.8 degrees resolution to estimate a global ocean source of about 4 (1.2-6.8) Tg N yr(-1). The wide range of uncertainty in the source estimate arises mainly from uncertainties in the air-sea gas transfer coefficients and in the global extrapolation of the summertime-biased surface N2O data set. The strongest source is predicted from the 40-60 degrees S latitude band. Strong emissions also are predicted from the northern Pacific Ocean, the equatorial upwelling zone, and coastal upwelling zones occurring predominantly in the tropical northern hemisphere. High apparent oxygen utilization (AOU) at 100 m below the mixed layer is found to be correlated positively both to N2O production at depth and to the surface N2O anomaly. On the basis of these correlations, the expedition data are partitioned into two subsets associated with high and low AOU at depth. The zonally averaged monthly means in each subset are extrapolated to produce two latitude-by-month matrices in which monthly surface N2O is expressed as the deviation from the annual mean. Both matrices contain large uncertainties. The low-AOU matrix, which mainly includes surface N2O data from the North Atlantic and the subtropical gyres, suggests many regions with positive summer deviations and negative winter deviations, consistent with a seasonal cycle predominantly driven by seasonal heating and cooling of the surface ocean. The high-AOU subset, which includes the regions most important to the global N2O ocean source, suggests some regions with positive winter deviations and negative summer deviations, consistent with a seasonal cycle predominantly driven by wintertime mixing of surface water with N2O-rich deep water. Coupled seasonal changes in gas transfer coefficients and surface N2O in these important source regions could strongly influence the global ocean source.