Nitrous oxide (N2O) is a long-lived greenhouse gas that affects atmospheric chemistry and climate. In this work, we use satellite measurements of N2O, ozone (O3), and temperature from the Aura Microwave Limb Sounder (MLS) instrument to calculate stratospheric loss of N2O, and thus its atmospheric lifetime. Using three chemistry transport models simulating the Aura period 2005–2017, we verify the stratospheric sink using MLS data and follow that loss signal down to the surface and compare with surface observations. Stratospheric loss has a strong seasonal cycle and is further modulated by the Quasi-Biennial Oscillation (QBO); these cycles are seen equally in both observations and the models. When filtered for interannual variability, the modeled surface signal is QBO-caused, and it reproduces the observed pattern, highlighting the potential role of the QBO in tropospheric chemistry and composition, as well as in model evaluation. The observed annual surface signal in the northern hemisphere matches well with the models run without emissions, indicating the annual cycle is driven mostly by stratosphere-troposphere exchange (STE) flux of N2O-depleted air and not surface N2O emissions. In the southern hemisphere (SH), all three models disagree and thus provide no guidance, except for indicating that modeling annual STE in the SH remains a major model uncertainty. Parallel model simulations of CFCl3, which has greater stratospheric loss that N2O and possibly surreptitious emissions, show that its interannual variations parallel those of N2O, and thus the observed N2O variability can identify the stratospheric component of the observed CFCl3 variability.

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.

Nitrous oxide (N₂O), like carbon dioxide, is a long-lived greenhouse gas that accumulates in the atmosphere. Over the past 150 years, increasing atmospheric N₂O concentrations have contributed to stratospheric ozone depletion¹ and climate change², with the current rate of increase estimated at 2 per cent per decade. Existing national inventories do not provide a full picture of N₂O emissions, owing to their omission of natural sources and limitations in methodology for attributing anthropogenic sources. Here we present a global N₂O inventory that incorporates both natural and anthropogenic sources and accounts for the interaction between nitrogen additions and the biochemical processes that control N₂O emissions. We use bottom-up (inventory, statistical extrapolation of flux measurements, process-based land and ocean modelling) and top-down (atmospheric inversion) approaches to provide a comprehensive quantification of global N₂O sources and sinks resulting from 21 natural and human sectors between 1980 and 2016. Global N₂O emissions were 17.0 (minimum-maximum estimates: 12.2-23.5) teragrams of nitrogen per year (bottom-up) and 16.9 (15.9-17.7) teragrams of nitrogen per year (top-down) between 2007 and 2016. Global human-induced emissions, which are dominated by nitrogen additions to croplands, increased by 30% over the past four decades to 7.3 (4.2-11.4) teragrams of nitrogen per year. This increase was mainly responsible for the growth in the atmospheric burden. Our findings point to growing N₂O emissions in emerging economies-particularly Brazil, China and India. Analysis of process-based model estimates reveals an emerging N₂O-climate feedback resulting from interactions between nitrogen additions and climate change. The recent growth in N₂O emissions exceeds some of the highest projected emission scenarios^3,4, underscoring the urgency to mitigate N₂O emissions.