Exploring causes of interannual variability in the seasonal cycles of tropospheric nitrous oxide

Abstract

Seasonal cycles in the mixing ratios of tropospheric nitrous oxide (N[subscript 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[subscript 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[subscript 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[subscript 2]O monthly means are correlated with polar spring lower stratospheric temperature in months preceding the N[subscript 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[subscript 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[subscript 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[subscript 2]O seasonal cycles suggests that, at sites remote from local sources, surface N[subscript 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[subscript 2]O that is of particular importance in the extratropical Southern Hemisphere, where it competes with the biological ocean source signal.