The Modeled Seasonal Cycles of Surface N2O Fluxes and Atmospheric N2O

Abstract

Nitrous oxide (N₂O) is a greenhouse gas and stratospheric ozone-depleting substance 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 eight remote air sampling sites for modern and pre-industrial periods. Models show general agreement on the seasonal phasing of zonal-average N₂O fluxes for most sites, but seasonal peak-to-peak amplitudes differ several-fold across models. The modeled seasonal amplitude of surface aN₂O ranges from 0.25 to 0.80 ppb (interquartile ranges 21%–52% of median) for land, 0.14–0.25 ppb (17%–68%) for ocean, and 0.28–0.77 ppb (23%–52%) for combined flux contributions. The observed seasonal amplitude ranges from 0.34 to 1.08 ppb for these sites. The stratospheric contributions to aN₂O, inferred by the difference between the surface-troposphere model and observations, show 16%–126% larger amplitudes and minima delayed by ∼1 month compared to Northern Hemisphere site observations. Land fluxes and their seasonal amplitude have increased since the pre-industrial era and are projected to grow further under anthropogenic activities. Our results demonstrate the increasing importance of land fluxes for aN₂O seasonality. Considering the large model spread, in situ aN₂O observations and atmospheric transport-chemistry models will provide opportunities for constraining terrestrial and oceanic biosphere models, critical for projecting carbon-nitrogen cycles under ongoing global warming.