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This is a repository copy of Acceleration of global N2O emissions seen from two decades of atmospheric inversion.

The Lagrangian particle dispersion model FLEX-PART in its original version in the mid-1990s was designed for calculating the long-range and mesoscale dispersion of hazardous substances from point sources, such as those released after an accident in a nuclear power plant. Over the past decades, the model has evolved into a comprehensive tool for multi-scale atmospheric transport modeling and analysis and has attracted a global user community. Its application fields have been extended to a large range of atmospheric gases and aerosols, e.g., greenhouse gases, short-lived climate forcers like black carbon and volcanic ash, and it has also been used to study the atmospheric branch of the water cycle. Given suitable meteorological input data, it can be used for scales from dozens of meters to global. In particular, inverse modeling based on source-receptor relationships from FLEXPART has become widely used. In this paper, we present FLEXPART version 10.4, which works with meteorological input data from the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecast System (IFS) and data from the United States National Cen-ters of Environmental Prediction (NCEP) Global Forecast System (GFS). Since the last publication of a detailed FLEX-PART description (version 6.2), the model has been improved in different aspects such as performance, physicochemical parameterizations, input/output formats, and available preprocessing and post-processing software. The model code has also been parallelized using the Message Passing Interface (MPI). We demonstrate that the model scales well up to using 256 processors, with a parallel efficiency greater than 75 % for up to 64 processes on multiple nodes in runs with very large numbers of particles. The deviation from 100 % efficiency is almost entirely due to the remaining nonparallelized parts of the code, suggesting large potential for further speedup. A new turbulence scheme for the convective boundary layer has been developed that considers the skewness in the vertical velocity distribution (updrafts and downdrafts) and vertical gradients in air density. FLEXPART is the only model available considering both effects, making it highly accurate for small-scale applications, e.g., to quantify dispersion in the vicinity of a point source. The wet deposi-Published by Copernicus Publications on behalf of the European Geosciences Union. 4956 I. Pisso et al.: FLEXPART version 10.4tion scheme for aerosols has been completely rewritten and a new, more detailed gravitational settling parameterization for aerosols has also been implemented. FLEXPART has had the option of running backward in time from atmospheric concentrations at receptor locations for many years, but this has now been extended to also work for deposition values and may become useful, for instance, for the interpretation of ice core measurements. To our knowledge, to date FLEX-PART is the only model with that capability. Furthermore, the temporal variation and temperature dependence of chemical reactions with ...

Our understanding and quantification of global soil nitrous oxide (N2O) emissions and the underlying processes remain largely uncertain. Here, we assessed the effects of multiple anthropogenic and natural factors, including nitrogen fertilizer (N) application, atmospheric N deposition, manure N application, land cover change, climate change, and rising atmospheric CO2 concentration, on global soil N2O emissions for the period 1861–2016 using a standard simulation protocol with seven process‐based terrestrial biosphere models. Results suggest global soil N2O emissions have increased from 6.3 ± 1.1 Tg N2O‐N/year in the preindustrial period (the 1860s) to 10.0 ± 2.0 Tg N2O‐N/year in the recent decade (2007–2016). Cropland soil emissions increased from 0.3 Tg N2O‐N/year to 3.3 Tg N2O‐N/year over the same period, accounting for 82% of the total increase. Regionally, China, South Asia, and Southeast Asia underwent rapid increases in cropland N2O emissions since the 1970s. However, US cropland N2O emissions had been relatively flat in magnitude since the 1980s, and EU cropland N2O emissions appear to have decreased by 14%. Soil N2O emissions from predominantly natural ecosystems accounted for 67% of the global soil emissions in the recent decade but showed only a relatively small increase of 0.7 ± 0.5 Tg N2O‐N/year (11%) since the 1860s. In the recent decade, N fertilizer application, N deposition, manure N application, and climate change contributed 54%, 26%, 15%, and 24%, respectively, to the total increase. Rising atmospheric CO2 concentration reduced soil N2O emissions by 10% through the enhanced plant N uptake, while land cover change played a minor role. Our estimation here does not account for indirect emissions from soils and the directed emissions from excreta of grazing livestock. To address uncertainties in estimating regional and global soil N2O emissions, this study recommends several critical strategies for improving the process‐based simulations.

43Nitrous oxide (N2O) is an important greenhouse gas (GHG) and also an ozone-depleting