A new aerosol wet removal scheme for the Lagrangian particle model FLEXPART v10

A new, more physically based wet removal scheme for aerosols has been implemented in the Lagrangian particle dispersion model FLEXPART. It uses three-dimensional cloud water fields from the European Centre for MediumRange Weather Forecasts (ECMWF) to determine cloud extent and distinguishes between in-cloud and below-cloud scavenging. The new in-cloud nucleation scavenging depends on cloud water phase (liquid, ice or mixed-phase), based on the aerosol's prescribed efficiency to serve as ice crystal nuclei and liquid water nuclei, respectively. The impaction scavenging scheme now parameterizes below-cloud removal as a function of aerosol particle size and precipitation type (snow or rain) and intensity. Sensitivity tests with the new scavenging scheme and comparisons with observational data were conducted for three distinct types of primary aerosols, which pose different challenges for modeling wet scavenging due to their differences in solubility, volatility and size distribution: (1) Cs-137 released during the Fukushima nuclear accident attached mainly to highly soluble sulphate aerosol particles, (2) black carbon (BC) aerosol particles, and (3) mineral dust. Calculated e-folding lifetimes of accumulation mode aerosols for these three aerosol types were 11.7, 16.0, and 31.6 days respectively, when well mixed in the atmosphere. These are longer lifetimes than those obtained by the previous removal schem, and, for mineral dust in particular, primarily result from very slow in-cloud removal, which globally is the primary removal mechanism for these accumulation mode particles. Calculated e-folding lifetimes in FLEXPART also have a strong size dependence, with the longest lifetimes found for the accumulation-mode aerosols. For example, for dust particles emitted at the surface the lifetimes were 13.8 days for particles with 1 aem diameter and a few hours for 10 aem particles. A strong size dependence in below-cloud scavenging, combined with increased dry removal, is the primary reason for the shorter lifetimes of the larger particles. The most frequent removal is in-cloud scavenging (85% of all scavenging events) but it occurs primarily in the free troposphere, while below-cloud removal is more frequent below 1000m (52% of all events) and can be important for the initial fate of species emitted at the surface, such as those examined here. For assumed realistic in-cloud removal efficiencies, both BC and sulphate have a slight overestimation of observed atmospheric concentrations (a factor of 1.6 and 1.2 respectively). However, this overestimation is largest close to the sources and thus appears more related to overestimated emissions rather than underestimated removal. The new aerosol wet removal scheme of FLEXPART incorporates more realistic information about clouds and aerosol properties and it compares better with both observed lifetimes and concentration than the old scheme.Peer reviewe

Modelling the 2021 East Asia super dust storm using FLEXPART and FLEXDUST and its comparison with reanalyses and observations

The 2021 East Asia sandstorm began from the Eastern Gobi desert steppe in Mongolia on March 14, and later spread to northern China and the Korean Peninsula. It was the biggest sandstorm to hit China in a decade, causing severe air pollution and a significant threat to human health. Capturing and predicting such extreme events is critical for society. The Lagrangian particle dispersion model FLEXPART and the associated dust emission model FLEXDUST have been recently developed and applied to simulate global dust cycles. However, how well the model captures Asian dust storm events remains to be explored. In this study, we applied FLEXPART to simulate the recent 2021 East Asia sandstorm, and evaluated its performance comparing with observation and observation-constrained reanalysis datasets, such as the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) and CAMS global atmospheric composition forecasts (CAMS-F). We found that the default setting of FLEXDUST substantially underestimates the strength of dust emission and FLEXPART modelled dust concentration in this storm compared to that in MERRA-2 and CAMS-F. An improvement of the parametrization of bare soil fraction, topographical scaling, threshold friction velocity and vertical dust flux scheme based on Kok et al. (Atmospheric Chemistry and Physics, 2014, 14, 13023-13041) in FLEXDUST can reproduce the strength and spatio-temporal pattern of the dust storm comparable to MERRA-2 and CAMS-F. However, it still underestimates the observed spike of dust concentration during the dust storm event over northern China, and requires further improvement in the future. The improved FLEXDUST and FLEXPART perform better than MERRA-2 and CAMS-F in capturing the observed particle size distribution of dust aerosols, highlighting the importance of using more dust size bins and size-dependent parameterization for dust emission, and dry and wet deposition schemes for modelling the Asian dust cycle and its climatic feedbacks.Peer reviewe

The consolidated European synthesis of CH4 and N2O emissions for the European Union and United Kingdom : 1990-2017

Reliable quantification of the sources and sinks of greenhouse gases, together with trends and uncertainties, is essential to monitoring the progress in mitigating anthropogenic emissions under the Paris Agreement. This study provides a consolidated synthesis of CH4 and N2O emissions with consistently derived state-of-the-art bottom-up (BU) and top-down (TD) data sources for the European Union and UK (EU27 C UK). We integrate recent emission inventory data, ecosystem process-based model results and inverse modeling estimates over the period 1990-2017. BU and TD products are compared with European national greenhouse gas inventories (NGHGIs) reported to the UN climate convention UNFCCC secretariat in 2019. For uncertainties, we used for NGHGIs the standard deviation obtained by varying parameters of inventory calculations, reported by the member states (MSs) following the recommendations of the IPCC Guidelines. For atmospheric inversion models (TD) or other inventory datasets (BU), we defined uncertainties from the spread between different model estimates or model-specific uncertainties when reported. In comparing NGHGIs with other approaches, a key source of bias is the activities included, e.g., anthropogenic versus anthropogenic plus natural fluxes. In inversions, the separation between anthropogenic and natural emissions is sensitive to the geospatial prior distribution of emissions. Over the 2011-2015 period, which is the common denominator of data availability between all sources, the anthropogenic BU approaches are directly comparable, reporting mean emissions of 20.8 TgCH(4) yr (-1) (EDGAR v5.0) and 19.0 TgCH(4) yr(-1) (GAINS), consistent with the NGHGI estimates of 18.9 +/- 1.7 TgCH(4) yr(-1). The estimates of TD total inversions give higher emission estimates, as they also include natural emissions. Over the same period regional TD inversions with higher-resolution atmospheric transport models give a mean emission of 28.8 TgCH(4) yr(-1). Coarser-resolution global TD inversions are consistent with regional TD inversions, for global inversions with GOSAT satellite data (23.3 TgCH(4) yr(-1)) and surface network (24.4 TgCH(4) yr (-1)). The magnitude of natural peatland emissions from the JSBACH-HIMMELI model, natural rivers and lakes emissions, and geological sources together account for the gap between NGHGIs and inversions and account for 5.2 TgCH(4) yr(-1). For N2O emissions, over the 2011-2015 period, both BU approaches (EDGAR v5.0 and GAINS) give a mean value of anthropogenic emissions of 0.8 and 0.9 TgN(2)Oyr(-1), respectively, agreeing with the NGHGI data (0.9 0.6 TgN(2)Oyr(-1)). Over the same period, the average of the three total TD global and regional inversions was 1.3 +/- 0.4 and 1.3 +/- 0.1 TgN(2)Oyr(-1), respectively. The TD and BU comparison method defined in this study can be operationalized for future yearly updates for the calculation of CH4 and N2O budgets both at the EU CUK scale and at the national scale.Peer reviewe

The consolidated European synthesis of CH4 and N2O emissions for the European Union and United Kingdom : 1990-2019

Funding Information: We thank Aurélie Paquirissamy, Géraud Moulas and the ARTTIC team for the great managerial support offered during the project. FAOSTAT statistics are produced and disseminated with the support of its member countries to the FAO regular budget. Annual, gap-filled and harmonized NGHGI uncertainty estimates for the EU and its member states were provided by the EU GHG inventory team (European Environment Agency and its European Topic Centre on Climate change mitigation). Most top-down inverse simulations referred to in this paper rely for the derivation of optimized flux fields on observational data provided by surface stations that are part of networks like ICOS (datasets: 10.18160/P7E9-EKEA , Integrated Non-CO Observing System, 2018a, and 10.18160/B3Q6-JKA0 , Integrated Non-CO Observing System, 2018b), AGAGE, NOAA (Obspack Globalview CH: 10.25925/20221001 , Schuldt et al., 2017), CSIRO and/or WMO GAW. We thank all station PIs and their organizations for providing these valuable datasets. We acknowledge the work of other members of the EDGAR group (Edwin Schaaf, Jos Olivier) and the outstanding scientific contribution to the VERIFY project of Peter Bergamaschi. Timo Vesala thanks ICOS-Finland, University of Helsinki. The TM5-CAMS inversions are available from https://atmosphere.copernicus.eu (last access: June 2022); Arjo Segers acknowledges support from the Copernicus Atmosphere Monitoring Service, implemented by the European Centre for Medium-Range Weather Forecasts on behalf of the European Commission (grant no. CAMS2_55). This research has been supported by the European Commission, Horizon 2020 Framework Programme (VERIFY, grant no. 776810). Ronny Lauerwald received support from the CLand Convergence Institute. Prabir Patra received support from the Environment Research and Technology Development Fund (grant no. JPMEERF20182002) of the Environmental Restoration and Conservation Agency of Japan. Pierre Regnier received financial support from the H2020 project ESM2025 – Earth System Models for the Future (grant no. 101003536). David Basviken received support from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (METLAKE, grant no. 725546). Greet Janssens-Maenhout received support from the European Union's Horizon 2020 research and innovation program (CoCO, grant no. 958927). Tuula Aalto received support from the Finnish Academy (grants nos. 351311 and 345531). Sönke Zhaele received support from the ERC consolidator grant QUINCY (grant no. 647204).Peer reviewedPublisher PD

Seasonal simulation of drifting snow sublimation in Alpine terrain

We estimate seasonal drifting snow sublimation at a study site in the Swiss Alps with the numerical model Alpine3D using external wind fields from the Advanced Regional Prediction System on a high-resolution grid (10 m). Novel in the field of snow transport modeling, the transport module of Alpine3D accounts for the feedbacks among drifting snow sublimation, snow concentration, temperature, and humidity of the air in three dimensions. Due to these feedbacks, drifting snow sublimation is a self-limiting process. Model results show that the domain averaged drifting snow sublimation over a season is small (about 0.1% of precipitation) but spatially highly variable. Simulation results show strongest seasonal reduction of snow amount by 1.8% due to drifting snow sublimation in a leeward slope during SE wind. This can be explained by the generally warmer and dryer conditions during events with SE wind. In the Wannengrat study area, which covers typical alpine terrain, drifting snow sublimation is thus only significant locally or on short time scales. Note that we only consider drifting and blowing snow in the absence of concurrent precipitation. Furthermore, our results show that drifting snow sublimation is much smaller than surface sublimation in this area. Citation: Groot Zwaaftink, C. D., R. Mott, and M. Lehning (2013), Seasonal simulation of drifting snow sublimation in Alpine terrain, Water Resour. Res., 49, 1581-1590, doi: 10.1002/wrcr.20137

A new aerosol wet removal scheme for the Lagrangian particle model FLEXPART

A new and more physically based treatment of how removal by precipitation is calculated by FLEXPART is introduced, to take into account more aspects of aerosol diversity. Also new, is the definition of clouds and cloud properties. Results from simulations show good agreement with observed atmospheric concentrations for distinctly different aerosols. Atmospheric lifetimes were found to vary from a few hours (large aerosol particles) up to a month (small non-soluble)

Effects of extreme meteorological conditions in 2018 on European methane emissions estimated using atmospheric inversions

The effect of the 2018 extreme meteorological conditions in Europe on methane (CH4) emissions is examined using estimates from four atmospheric inversions calculated for the period 2005–2018. For most of Europe, we find no anomaly in 2018 compared to the 2005–2018 mean. However, we find a positive anomaly for the Netherlands in April, which coincided with positive temperature and soil moisture anomalies suggesting an increase in biogenic sources. We also find a negative anomaly for the Netherlands for September–October, which coincided with a negative anomaly in soil moisture, suggesting a decrease in soil sources. In addition, we find a positive anomaly for Serbia in spring, summer and autumn, which coincided with increases in temperature and soil moisture, again suggestive of changes in biogenic sources, and the annual emission for 2018 was 33 ± 38% higher than the 2005–2017 mean. These results indicate that CH4 emissions from areas where the natural source is thought to be relatively small can still vary due to meteorological conditions. At the European scale though, the degree of variability over 2005–2018 was small, and there was negligible impact on the annual CH4 emissions in 2018 despite the extreme meteorological conditions. This article is part of a discussion meeting issue ‘Rising methane: is warming feeding warming? (part 2)’

Three-dimensional methane distribution simulated with FLEXPART 8-CTM-1.1 constrained with observation data

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The consolidated European synthesis of CH4 and N2O emissions for EU27 and UK: 1990–2020

Knowledge of the spatial distribution of the fluxes of greenhouse gases and their temporal variability as well as flux attribution to natural and anthropogenic processes is essential to monitoring the progress in mitigating anthropogenic emissions under the Paris Agreement and to inform its Global Stocktake. This study provides a consolidated synthesis of CH4 and N2O emissions using bottom-up (BU) and top-down (TD) approaches for the European Union and UK (EU27+UK) and updates earlier syntheses (Petrescu et al., 2020, 2021). The work integrates updated emission inventory data, process-based model results, data-driven sector model results, inverse modelling estimates, and extends the previous period 1990–2017 to 2020. BU and TD products are compared with European National GHG Inventories (NGHGI) reported by Parties under the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. The uncertainties of NGHGIs were evaluated using the standard deviation obtained by varying parameters of inventory calculations, reported by the EU Member States following the guidelines of the Intergovernmental Panel on Climate Change (IPCC) and harmonized by gap-filling procedures. Variation in estimates produced with other methods, such as atmospheric inversion models (TD) or spatially disaggregated inventory datasets (BU), arise from diverse sources including within-model uncertainty related to parameterization as well as structural differences between models. By comparing NGHGIs with other approaches, the activities included are a key source of bias between estimates e.g. anthropogenic and natural fluxes, which, in atmospheric inversions are sensitive to the prior geospatial distribution of emissions. For CH4 emissions, over the updated 2015–2019 period, which covers a sufficiently robust number of overlapping estimates, and most importantly the NGHGIs, the anthropogenic BU approaches are directly comparable, accounting for mean emissions of 20.5 Tg CH4 yr−1 (EDGAR v5v6.0, last year 2018) and 18.4 Tg CH4 yr−1 (GAINS, 2015), close to the NGHGI estimates of 17.5 ± 2.1 Tg CH4 yr−1. TD inversions estimates give higher emission estimates, as they also detect natural emissions. Over the same period, high resolution regional TD inversions report a mean emission of 34 Tg CH4 yr−1. Coarser-resolution global-scale TD inversions result in emission estimates of 23 Tg CH4 yr−1 and 24 Tg CH4 yr−1 inferred from GOSAT and surface (SURF) network atmospheric measurements, respectively. The magnitude of natural peatland and mineral soils emissions from the JSBACH-HIMMELI model, natural rivers, lakes and reservoirs emissions, geological sources and biomass burning together could account for the gap between NGHGI and inversions and account for 8 Tg CH4 yr−1. For N2O emissions, over the 2015–2019 period, both BU products (EDGAR v5v6.0 and GAINS) report a mean value of anthropogenic emissions of 0.9 Tg N2O yr−1, close to the NGHGI data (0.8 ± 55 % Tg N2O yr−1). Over the same period, the mean of TD global and regional inversions was 1.4 Tg N2O yr−1 (excluding TOMCAT which reported no data). The TD and BU comparison method defined in this study can be "operationalized" for future annual updates for the calculation of CH4 and N2O budgets at the national and EU27+UK scales. Future comparability will be enhanced with further steps involving analysis at finer temporal resolutions and estimation of emissions over intra-annual timescales, of great importance for CH4 and N2O, which may help identify sector contributions to divergence between prior and posterior estimates at the annual/inter-annual scale. Even if currently comparison between CH4 and N2O inversions estimates and NGHGIs is highly uncertain because of the large spread in the inversion results, TD inversions inferred from atmospheric observations represent the most independent data against which inventory totals can be compared. With anticipated improvements in atmospheric modelling and observations, as well as modelling of natural fluxes, TD inversions may arguably emerge as the most powerful tool for verifying emissions inventories for CH4, N2O and other GHGs. The referenced datasets related to figures are visualized at https://doi.org/10.5281/zenodo.6992472 (Petrescu et al., 2022)