Qing Sun

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Nitrous oxide (N2O) is a greenhouse gas and an ozone-depleting agent with large and growing anthropogenic emissions. Previous studies identified the influx of N2O-depleted air from the stratosphere to partly cause the seasonality in tropospheric N2O (aN2O), but other contributions remain unclear. Here we combine surface fluxes from eight land and four ocean models from phase 2 of the Nitrogen/N2O Model Intercomparison Project with tropospheric transport modeling to simulate aN2O at the air sampling sites: Alert, Barrow, Ragged Point, Samoa, Ascension Island, and Cape Grim for the modern and preindustrial periods. Models show general agreement on the seasonal phasing of zonal-average N2O fluxes for most sites, but, seasonal peak-to-peak amplitudes differ severalfold across models. After transport, the seasonal amplitude of surface aN2O ranges from 0.25 to 0.80 ppb (interquartile ranges 21-52% of median) for land, 0.14 to 0.25 ppb (19-42%) for ocean, and 0.13 to 0.76 ppb (26-52%) for combined flux contributions. The observed range is 0.53 to 1.08 ppb. The stratospheric contributions to aN2O, inferred by the difference between surface-troposphere model and observations, show 36-126% larger amplitudes and minima delayed by ~1 month compared to Northern Hemisphere site observations. Our results demonstrate an increasing importance of land fluxes for aN2O seasonality, with land fluxes and their seasonal amplitude increasing since the preindustrial era and are projected to grow under anthropogenic activities. In situ aN2O observations and atmospheric transport-chemistry models will provide opportunities for constraining terrestrial and oceanic biosphere models, critical for projecting surface N2O sources under ongoing global warming.