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An operational multi-model forecasting system for air quality has been developed to provide air quality services for urban areas of China. The initial forecasting system included seven state-of-the-art computational models developed and executed in Europe and China (CHIMERE, IFS, EMEP MSC-W, WRF-Chem-MPIM, WRF-Chem-SMS, LOTOS-EUROS and SILAMtest). Several other models joined the prediction system recently, but are not considered in the present analysis. In addition to the individual models, a simple multi-model ensemble was constructed by deriving statistical quantities such as the median and the mean of the predicted concentrations. The prediction system provides daily forecasts and observational data of surface ozone, nitrogen dioxides and particulate matter for the 37 largest urban agglomerations in China (population higher than 3 million in 2010). These individual forecasts as well as the multi-model ensemble predictions for the next 72 hours are displayed as hourly outputs on a publicly accessible web site (www.marcopolo-panda.eu). In this paper, the performance of the predictions system (individual models and the multi-model ensemble) for the first operational year (April 2016 until June 2017) has been analysed through statistical indicators using the surface observational data reported at Chinese national monitoring stations. This evaluation aims to investigate a) the seasonal behavior, b) the geographical distribution and c) diurnal variations of the ensemble and model skills. Statistical indicators show that the ensemble product usually provides the best performance compared to the individual model forecasts. The ensemble product is robust even if occasionally some individual model results are missing. Overall and in spite of some discrepancies, the air quality forecasting system is well suited for the prediction of air pollution events and has the ability to provide alert warning (binary prediction) of air pollution events if bias corrections are applied to improve the ozone predictions. [ABSTRACT FROM AUTHOR]

An operational multi-model forecasting system for air quality including 9 different chemical transport models has been developed and is providing daily forecasts of ozone, nitrogen oxides, and particulate matter for the 37 largest urban areas of China (population higher than 3 million in 2010). These individual forecasts as well as the mean and median concentrations for the next 3 days are displayed on a publicly accessible web site (http://www.marcopolo-panda.eu). The paper describes the forecasting system and shows some selected illustrative examples of air quality predictions. It presents an inter-comparison of the different forecasts performed during a given period of time (1-15 March 2017), and highlights recurrent differences between the model output as well as systematic biases that appear in the median concentration values. Pathways to improve the forecasts by the multi-model system are suggested. [ABSTRACT FROM AUTHOR]

A Lagrangian particle dispersion model (FLEXPART CTM) is used to simulate global three-dimensional fields of trace gas abundance. These fields are constrained with surface observation data through nudging, a data assimilation method which relaxes model fields to observed values. Such fields are of interest to a variety of applications, such as inverse modelling, satellite retrievals and estimating global growth rates of greenhouse gases. Here, we apply this method to methane using 6 million model particles filling the global model domain. For each particle methane mass tendencies due to emissions based on several inventories, loss by reaction with OH, Cl, and O(¹D), as well as observation data nudging were calculated. Model particles were transported by mean, turbulent and convective transport driven by 1° x 1° ERA Interim meteorology. Nudging is applied at 79 surface stations, which are mostly included in the WDCGG database or JR-STATION network in Siberia. For simulations of one year (2013), we perform a sensitivity analysis to show how nudging settings affect modelled concentration fields. These are evaluated with a set of independent surface observations and with vertical profiles in North America (NOAA/ESRL) and Siberia (YAK-AEROSIB and NIES). FLEXPART CTM results are also compared to simulations from the global Eulerian model, TM5, based on optimized fluxes. Results show that nudging strongly improves modelled methane near the surface, not only at the nudging locations, but also at independent stations. Mean bias at all surface locations could be reduced from over 20 ppb to less than 5 ppb through nudging. Near the surface, FLEXPART CTM, including nudging, appears better able to capture methane molar mixing ratios than TM5 with optimized fluxes, based on a larger bias of over 13 ppb in TM5 simulations. The vertical profiles indicate that nudging affects model methane at high altitudes, yet leads to very little improvement in the model results there. Averaged from 19 aircraft profile locations in North America and Siberia, root-mean square error (RMSE) changes only from 16.3 to 15.7 ppb through nudging, while the mean absolute bias increases from 5.3 to 8.2 ppb. The performance for vertical profiles is thereby similar to TM5 simulations based on TM5 optimized fluxes where we found a bias of 5 ppb and RMSE of 15.9 ppb. With this rather simple model setup, we thus provide three-dimensional methane fields suitable for use as boundary conditions in regional inverse modelling, as prior information for satellite retrievals, and for more accurate estimation of mean mixing ratios and growth rates. The method should also be applicable to other long-lived trace gases. [ABSTRACT FROM AUTHOR]

Biodiversity is strongly affected by the deposition of nitrogen and sulfur on terrestrial ecosystems. In this paper we present new quantitative estimates of the deposition of atmospheric nitrogen to ecosystems across Germany. The methodology combines prognostic and empirical modelling to establish wet deposition fluxes and land use dependent dry and occult deposition fluxes. On average, the nitrogen deposition in Germany was estimated to be 1057 eq ha-1 yr-1. The deposition maps show considerable variability across the German territory with highest deposition on forest ecosystems in or near the main agricultural and industrial areas. The accumulated deposition over Germany of this study is systematically lower (27 %) than provided in earlier studies. The main reasons are an improved wet deposition estimation and the consolidation of improved process descriptions in the LOTOS-EUROS chemistry transport model. The presented deposition estimates show a better agreement with results obtained by integrated monitoring and deposition modelling by EMEP than the earlier results. Through comparison of the new deposition distributions with critical load maps it is estimated that 70 % of the ecosystems in Germany receive too much nitrogen. [ABSTRACT FROM AUTHOR]

In this study, we investigate a strategy to accelerate the data assimilation (DA) algorithm. Based on evaluations of the computational time, the analysis step of the assimilation turns out to be the most expensive part. After a study of the characteristics of the ensemble ash state, we propose a mask-state algorithm which records the sparsity information of the full ensemble state matrix and transforms the full matrix into a relatively small one. This will reduce the computational cost in the analysis step. Experimental results show the mask-state algorithm significantly speeds up the analysis step. Subsequently, the total amount of computing time for volcanic ash DA is reduced to an acceptable level. The mask-state algorithm is generic and thus can be embedded in any ensemble-based DA framework. Moreover, ensemble-based DA with the mask-state algorithm is promising and flexible, because it implements exactly the standard DA without any approximation and it realizes the satisfying performance without any change in the full model. [ABSTRACT FROM AUTHOR]

Using data assimilation (DA) to improve model forecast accuracy is a powerful approach that requires available observations. Infrared satellite measurements of volcanic ash mass loadings are often used as input observations for the assimilation scheme. However, because these primary satellite-retrieved data are often two-dimensional (2-D) and the ash plume is usually vertically located in a narrow band, directly assimilating the 2-D ash mass loadings in a three-dimensional (3-D) volcanic ash model (with an integral observational operator) can usually introduce large artificial/spurious vertical correlations. In this study, we look at an approach to avoid the artificial vertical correlations by not involving the integral operator. By integrating available data of ash mass loadings and cloud top heights, as well as data-based assumptions on thickness, we propose a satellite observational operator (SOO) that translates satellite-retrieved 2-D volcanic ash mass loadings to 3-D concentrations. The 3-D SOO makes the analysis step of assimilation comparable in the 3-D model space. Ensemble-based DA is used to assimilate the extracted measurements of ash concentrations. The results show that satellite DA with SOO can improve the estimate of volcanic ash state and the forecast. Comparison with both satellite-retrieved data and aircraft in situ measurements shows that the effective duration of the improved volcanic ash forecasts for the distal part of the Eyjafjallajökull volcano is about 6 h. [ABSTRACT FROM AUTHOR]

The forecast accuracy of distal volcanic ash clouds is important for providing valid aviation advice during volcanic ash eruption. However, because the distal part of volcanic ash plume is far from the volcano, the influence of eruption information on this part becomes rather indirect and uncertain, resulting in inaccurate volcanic ash forecasts in these distal areas. In our approach, we use real-life aircraft in situ observations, measured in the northwestern part of Germany during the 2010 Eyjafjallajökull eruption, in an ensemble-based data assimilation system combined with a volcanic ash transport model to investigate the potential improvement on the forecast accuracy with regard to the distal volcanic ash plume. We show that the error of the analyzed volcanic ash state can be significantly reduced through assimilating real-life in situ measurements. After a continuous assimilation, it is shown that the aviation advice for Germany, the Netherlands and Luxembourg can be significantly improved. We suggest that with suitable aircrafts measuring once per day across the distal volcanic ash plume, the description and prediction of volcanic ash clouds in these areas can be greatly improved. [ABSTRACT FROM AUTHOR]

Data assimilation is a powerful tool that requires available observations to improve model forecast accuracy. Infrared satellite measurements of volcanic ash mass loadings are often used as input observations into the assimilation scheme. However, these satellite-retrieved data are often two-dimensional (2D), and cannot be easily combined with a three-dimensional (3D) volcanic ash model to continuously improve the volcanic ash state in a data assimilation system. By integrating available data including ash mass loadings, cloud top heights and thickness information, we propose a satellite observational operator (SOO) that translates satellite-retrieved 2D volcanic ash mass loadings to 3D concentrations at the top layer of the ash cloud. Ensemble-based data assimilation is used to continuously assimilate the extracted measurements of ash concentrations. The results show that satellite data assimilation can force the volcanic ash state to match the satellite observations, and that it improves the forecast of the ash state. Comparison with highly accurate aircraft in-situ measurements shows that the effective duration of the improved volcanic ash forecasts is about a half day. It is shown that an effective half-day ash forecast significantly improves the quality of the advice given to aviation over continental Europe. [ABSTRACT FROM AUTHOR]

In this study, we investigate strategies for accelerating data assimilation on volcanic ash forecasts. Based on evaluations of computational time, the analysis step of the assimilation is evaluated as the most expensive part. After a careful study on the characteristics of the ensemble ash state, we propose a mask-state algorithm which records the sparsity information of the full ensemble state matrix and transforms the full matrix into a relatively small one. This will reduce the computational cost in the analysis step. Experimental results show the mask-state algorithm significantly speeds up the expensive analysis step. Subsequently, the total amount of computing time for volcanic ash data assimilation is reduced to an acceptable level, which is important for providing timely and accurate aviation advices. The mask-state algorithm is generic and thus can be embedded in any ensemble-based data assimilation framework. Moreover, ensemble-based data assimilation with the mask-state algorithm is promising and flexible, because it implements exactly the standard data assimilation without any approximation and it realizes the satisfying performance without any change of the full model. [ABSTRACT FROM AUTHOR]

Meteorological fields calculated by Numerical Weather Prediction (NWP) Models drive offline Chemical Transport Models (CTM) to solve the transport, chemical reactions, and atmospheric interaction over the geographical domain of interest. In this way, forecasts and (re-)analyses provided by NWP can be used for air quality forecasting, climate modeling, and environmental studies. The more precise the meteorological input data represents the atmospheric dynamics, the better the CTM represents pollutant transport, mixing, and the subsequent impact on surface air quality. HARMONIE (HIRLAM ALADIN Research on Mesoscale Operational NWP in Euromed) is a state-of-the-art non-hydrostatic NWP community model used at several European weather agencies to forecast weather at the local and/or regional scale. In this work, the HARMONIE WINS50 (cycle 43 cy43) reanalysis data set at a resolution of 0.025° ×0.025° covering an area surrounding the North Sea for the years 2019-2021 was offline coupled to the state-of-the-art model LOTOS-EUROS (v2.2.002), which is a CTM that is one of the members of the Copernicus Atmosphere Monitoring Service (CAMS), an ensemble of CTMs that is used to produce operational air quality forecasts over Europe and at a higher resolution also over the Netherlands. The impact on simulated NO2 concentrations of using meteorological fields from HARMONIE in LOTOS-EUROS compared to the use of fields from ECMWF (here used at 0.7°×0.7°) is evaluated against ground-level sensors and TROPOMI tropospheric NO2 vertical columns. Furthermore, the difference between crucial meteorological input parameters such as the boundary layer height and the vertical diffusion coefficient between the hydrostatic (ECMWF) and non-hydrostatic (HARMONIE) model fields is studied, and the vertical profiles of temperature, humidity, and wind are evaluated against meteorological vertical profile observations at Cabauw in The Netherlands. The results of these first evaluations of the LOTOS-EUROS model performance in both configurations are used to investigate current uncertainties in air quality forecasting in relation to driving meteorological parameters and to assess the potential for improvements in high-resolution air quality forecasting episodes based on the HAR MONIE NWP model. [ABSTRACT FROM AUTHOR]

Statistical methods, particularly machine learning models, have gained significant popularity in air quality predictions. These prediction models are commonly trained using the historical measurement datasets independently collected at the environmental monitoring stations and their operational forecasts in advance using inputs of the real-time ambient pollutant observations. Therefore, these high-quality machine learning models only provide site-available predictions and cannot solely be used as the operational forecast. In contrast, deterministic chemical transport models (CTMs), which simulate the full life cycles of air pollutants, provide predictions that are continuous in the 3D field. Despite their benefits, CTM predictions are typically biased, particularly on a fine scale, owing to the complex error sources due to the emission, transport, and removal of pollutants. In this study, we proposed a fusion of site-available machine learning prediction, which is from our regional feature selection-based machine learning model (RFSML v1.0), and a CTM prediction. Compared to the normal pure machine learning model, the fusion system provides a gridded prediction with relatively high accuracy. The prediction fusion was conducted using the Bayesian-theory-based ensemble Kalman filter (EnKF). Background error covariance was an essential part in the assimilation process. Ensemble CTM predictions driven by the perturbed emission inventories were initially used for representing their spatial covariance statistics, which could resolve the main part of the CTM error. In addition, a covariance inflation algorithm was designed to amplify the ensemble perturbations to account for other model errors next to the uncertainty in emission inputs. Model evaluation tests were conducted based on independent measurements. Our EnKF-based prediction fusion presented superior performance compared to the pure CTM. Moreover, covariance inflation further enhanced the fused prediction, particularly in cases of severe underestimation. [ABSTRACT FROM AUTHOR]

In this work, we present the development of a 4D-Ensemble-Variational (4DEnVar) data assimilation technique to estimate NO x top-down emissions using the regional chemical transport model LOTOS-EUROS with the NO 2 observations from the TROPOspheric Monitoring Instrument (TROPOMI). The assimilation was performed for a domain in the northwest of South America centered over Colombia, and includes regions in Panama, Venezuela and Ecuador. In the 4DEnVar approach, the implementation of the linearized and adjoint model are avoided by generating an ensemble of model simulations and by using this ensemble to approximate the nonlinear model and observation operator. Emission correction parameters' locations were defined for positions where the model simulations showed significant discrepancies with the satellite observations. Using the 4DEnVar data assimilation method, optimal emission parameters for the LOTOS-EUROS model were estimated, allowing for corrections in areas where ground observations are unavailable and the region's emission inventories do not correctly reflect the current emissions activities. The analyzed 4DEnVar concentrations were compared with the ground measurements of one local air quality monitoring network and the data retrieved by the satellite instrument Ozone Monitoring Instrument (OMI). The assimilation had a low impact on NO 2 surface concentrations reducing the Mean Fractional Bias from 0.45 to 0.32, primordially enhancing the spatial and temporal variations in the simulated NO 2 fields. [ABSTRACT FROM AUTHOR]

The aim of this paper is to apply a new lane separation methodology for the maritime sector emissions attributed to the different vessel types and marine traffic loads in the Mediterranean and the Black Sea defined via the European Marine and Observation Data network (EMODnet), developed in 2016. This methodology is implemented for the first time on the Copernicus Atmospheric Monitoring Service Global Shipping (CAMS-GLOB-SHIP v2.1) nitrogen oxides (NOX) emissions inventory, on the Sentinel-5 Precursor Tropospheric Monitoring Instrument (TROPOMI) nitrogen dioxide (NO2) tropospheric vertical column densities, and on the LOTOS-EUROS (Long Term Ozone Simulation—European Operational Smog) CTM (chemical transport model) simulations. By applying this new EMODnet-based lane separation method to the CAMS-GLOB-SHIP v2.1 emission inventory, we find that cargo and tanker vessels account for approximately 80% of the total emissions in the Mediterranean, followed by fishing, passenger, and other vessel emissions with contributions of 8%, 7%, and 5%, respectively. Tropospheric NO2 vertical column densities sensed by TROPOMI for 2019 and simulated by the LOTOS-EUROS CTM have been successfully attributed to the major vessel activities in the Mediterranean; the mean annual NO2 load of the observations and the simulations reported for the entire maritime EMODnet-reported fleet of the Mediterranean is in satisfactory agreement, 1.26 ± 0.56 × 1015 molecules cm−2 and 0.98 ± 0.41 × 1015 molecules cm−2, respectively. The spatial correlation of the annual maritime NO2 loads of all vessel types between observation and simulation ranges between 0.93 and 0.98. On a seasonal basis, both observations and simulations show a common variability. The wintertime comparisons are in excellent agreement for the highest emitting sector, cargo vessels, with the observations reporting a mean load of 0.98 ± 0.54 and the simulations of 0.81 ± 0.45 × 1015 molecules cm−2 and correlation of 0.88. Similarly, the passenger sector reports 0.45 ± 0.49 and 0.39 ± 0.45 × 1015 molecules cm−2 respectively, with correlation of 0.95. In summertime, the simulations report a higher decrease in modelled tropospheric columns than the observations, however, still resulting in a high correlation between 0.85 and 0.94 for all sectors. These encouraging findings will permit us to proceed with creating a top-down inventory for NOx shipping emissions using S5P/TROPOMI satellite observations and a data assimilation technique based on the LOTOS-EUROS chemical transport model. [ABSTRACT FROM AUTHOR]

Statistical methods, particularly machine learning models, have gained significant popularity in air quality predictions. These prediction models are trained using the historical measurement datasets independently collected at the environmental monitoring stations, and their operational forecasts onward by the inputs of the real-time ambient pollutant observations. Therefore, these high-quality machine learning models only provide site-available predictions. In contrast, deterministic chemical transport models (CTM), which simulate the full life cycles of air pollutants, provide forecasts that are continuous in 3D field. However, owing to the complex error sources due to the emission, transport, and removal of pollutants, CTM forecasts are typically biased particularly in fine scale. In this study, we proposed a gridded prediction with high accuracy by fusing predictions from our recent regional-feature-selection machine learning prediction (RFSML v1.0) and a CTM forecast. The prediction fusion was conducted using the Bayesian theory-based ensemble Kalman filter (EnKF). Background error covari ance was an essential part in the assimilation process. Ensemble CTM predictions driven by the perturbed emission inventories were initially used for representing their spatial covariance statistics, which could resolve the main part of the CTM error. In addition, a covariance inflation algorithm was designed to amplify the ensemble perturbations to account for other model errors next to the uncertainty in emission inputs. Model evaluation tests were conducted based on independent measurements. Our EnKF-based prediction fusion presented significant improvements than the pure CTM. Moreover, covariance inflation further enhanced the fused prediction particularly in the cases of severe underestimation. [ABSTRACT FROM AUTHOR]

With the explosive growth of atmospheric data, machine learning models have achieved great success in air pollution forecasting because of their higher computational efficiency than the traditional chemical transport models. However, in previous studies, new prediction algorithms have only been tested at stations or in a small region; a large-scale air quality forecasting model remains lacking to date. Huge dimensionality also means that redundant input data may lead to increased complexity and therefore the over-fitting of machine learning models. Feature selection is a key topic in machine learning development, but it has not yet been explored in atmosphere-related applications. In this work, a regional feature selection-based machine learning (RFSML) system was developed, which is capable of predicting air quality in the short term with high accuracy at the national scale. Ensemble-Shapley additive global importance analysis is combined with the RFSML system to extract significant regional features and eliminate redundant variables at an affordable computational expense. The significance of the regional features is also explained physically. Compared with a standard machine learning system fed with relative features, the RFSML system driven by the selected key features results in superior interpretability, less training time, and more accurate predictions. This study also provides insights into the difference in interpretability among machine learning models (i.e., random forest, gradient boosting, and multi-layer perceptron models). [ABSTRACT FROM AUTHOR]

Accurately forecasting ozone levels that exceed specific thresholds is pivotal for mitigating adverse effects on both the environment and public health. However, predicting such ozone exceedances remains challenging due to the infrequent occurrence of high-concentration ozone data. This research, leveraging data from 57 German monitoring stations from 1999 to 2018, introduces an Enhanced Extreme Instance Augmentation Random Forest (EEIA-RF) approach that significantly improves the prediction of days when the maximum daily 8-hour average ozone concentrations exceed 120 μ g/m 3 . A pre-trained machine learning model is used to generate additional high-concentration data, which, combined with selectively reduced low-concentration data, forms a new dataset for training a refined model. This method achieved an improvement of at least 8% in the accuracy of predicting days with ozone exceedances across Germany. Our experiment underscores the approach's value in enhancing atmospheric modeling and supporting public health advisories and environmental policy-making related to ozone pollution. • The study introduce EEIA-RFM to enhance ozone exceedance prediction accuracy. • K-means clustering on data from 57 German stations for regional analysis. • EEIA-RFM outperforms traditional methods in forecasting ozone exceedances. [ABSTRACT FROM AUTHOR]

Monitoring the spatial distribution and trends in surface greenhouse gas (GHG) fluxes, as well as flux attribution to natural and anthropogenic processes, is essential to track progress under the Paris Agreement and to inform its global stocktake. This study updates earlier syntheses (Petrescu et al., 2020, 2021, 2023), provides a consolidated synthesis of CH 4 emissions using bottom-up (BU) and top-down (TD) approaches for the European Union (EU), and is expanded to include seven additional countries with large anthropogenic and/or natural emissions (the USA, Brazil, China, India, Indonesia, Russia, and the Democratic Republic of the Congo (DR Congo)). Our aim is to demonstrate the use of different emission estimates to help improve national GHG emission inventories for a diverse geographical range of stakeholders. We use updated national GHG inventories (NGHGIs) reported by Annex I parties under the United Nations Framework Convention on Climate Change (UNFCCC) in 2023 and the latest available biennial update reports (BURs) reported by non-Annex I parties. Comparing NGHGIs with other approaches highlights that different system boundaries are a key source of divergence. A key system boundary difference is whether anthropogenic and natural fluxes are included and, if they are, how fluxes belonging to these two sources are partitioned. Over the studied period, the total CH 4 emission estimates in the EU, the USA, and Russia show a steady decreasing trend since 1990, while for the non-Annex I emitters analyzed in this study, Brazil, China, India, Indonesia, and DR Congo, CH 4 emissions have generally increased. Quantitatively, in the EU the mean of 2015–2020 anthropogenic UNFCCC NGHGIs (15±1.8 Tg CH 4 yr -1) and the mean of the BU CH 4 emissions (17.8 (16–19) Tg CH 4 yr -1) generally agree on the magnitude, while inversions show higher emission estimates (medians of 21 (19–22) Tg CH 4 yr -1 and 24 (22–25) Tg CH 4 yr -1 for the three regional and six global inversions, respectively), as they include natural emissions, which for the EU were quantified at 6.6 Tg CH 4 yr -1 (Petrescu et al., 2023). Similarly, for the other Annex I parties in this study (the USA and Russia), the gap between the BU anthropogenic and total TD emissions is partly explained by the natural emissions. For the non-Annex I parties, anthropogenic CH 4 estimates from UNFCCC BURs show large differences compared to the other global-inventory-based estimates and even more compared to atmospheric ones. This poses an important potential challenge to monitoring the progress of the global CH 4 pledge and the global stocktake. Our analysis provides a useful baseline to prepare for the influx of inventories from non-Annex I parties as regular reporting starts under the enhanced transparency framework of the Paris Agreement. By systematically comparing the BU and TD methods, this study provides recommendations for more robust comparisons of available data sources and hopes to steadily engage more parties in using observational methods to complement their UNFCCC inventories, as well as considering their natural emissions. With anticipated improvements in atmospheric modeling and observations, as well as modeling of natural fluxes, future development needs to resolve knowledge gaps in the BU and TD approaches and to better quantify the remaining uncertainty. TD methods may emerge as a powerful tool to help improve NGHGIs of CH 4 emissions, but further confidence is needed in the comparability and robustness of the estimates. The referenced datasets related to figures are available at 10.5281/zenodo.12818506 (Petrescu et al., 2024). [ABSTRACT FROM AUTHOR]

In this work, we investigate the ability of a data assimilation technique and space-borne observations to quantify and monitor changes in nitrogen oxides (NOx) emissions over Northwestern Greece for the summers of 2018 and 2019. In this region, four lignite-burning power plants are located. The data assimilation technique, based on the Ensemble Kalman Filter method, is employed to combine space-borne atmospheric observations from the high spatial resolution Sentinel-5 Precursor (S5P) Tropospheric Monitoring Instrument (TROPOMI) and simulations using the LOTOS-EUROS Chemical Transport model. The Copernicus Atmosphere Monitoring Service-Regional European emissions (CAMS-REG, version 4.2) inventory based on the year 2015 is used as the a priori emissions in the simulations. Surface measurements of nitrogen dioxide (NO2) from air quality stations operating in the region are compared with the model surface NO2 output using either the a priori (base run) or the a posteriori (assimilated run) NOx emissions. Relative to the a priori emissions, the assimilation suggests a strong decrease in concentrations for the station located near the largest power plant, by 80% in 2019 and by 67% in 2018. Concerning the estimated annual a posteriori NOx emissions, it was found that, for the pixels hosting the two largest power plants, the assimilated run results in emissions decreased by ~40–50% for 2018 compared to 2015, whereas a larger decrease, of ~70% for both power plants, was found for 2019, after assimilating the space-born observations. For the same power plants, the European Pollutant Release and Transfer Register (E-PRTR) reports decreased emissions in 2018 and 2019 compared to 2015 (−35% and −38% in 2018, −62% and −72% in 2019), in good agreement with the estimated emissions. We further compare the a posteriori emissions to the reported energy production of the power plants during the summer of 2018 and 2019. Mean decreases of about −35% and−63% in NOx emissions are estimated for the two larger power plants in summer of 2018 and 2019, respectively, which are supported by similar decreases in the reported energy production of the power plants (~−30% and −70%, respectively). [ABSTRACT FROM AUTHOR]

Atmospheric inversions are used to constrain emissions of trace gases using atmospheric mole-fraction measurements. The four-dimensional variational (4DVAR) inversion approach allows optimization of emissions at a higher temporal and spatial resolution than ensemble or analytical approaches but provides limited opportunities for scalable parallelization because it is an iterative optimization method. Multidecadal variational inversions are needed to optimally extract information from the long measurement records of long-lived atmospheric trace gases like carbon dioxide and methane. However, the wall time needed – up to months – complicates these multidecadal inversions. The physical parallelization (PP) method introduced by Chevallier (2013) addresses this problem for carbon dioxide inversions by splitting the period of the chemical transport model into blocks and running them in parallel. Here, we present a new implementation of the PP method which is suitable for methane inversions accounting for the chemical sink of methane. The performance of the PP method is tested in an 11-year inversion using a TM5-4DVAR inversion setup that assimilates surface observations to optimize methane emissions at grid scale. Our PP implementation improves the wall time performance by a factor of 5 and shows excellent agreement with a full serial inversion in an identical configuration (global mean emissions difference =0.06% with an interannual variation correlation R=0.99 ; regional mean emission difference <5% and interannual variation R>0.94). The wall time improvement of the PP method increases with the size of the inversion period. The PP method is planned to be used in future releases of the Copernicus Atmosphere Monitoring Service (CAMS) multidecadal methane reanalysis. [ABSTRACT FROM AUTHOR]

The aim of this paper is to evaluate the surface concentration of nitrogen dioxide (NO2) inferred from the Sentinel-5 Precursor Tropospheric Monitoring Instrument (S5P/TROPOMI) NO2 tropospheric column densities over Central Europe for two time periods, summer 2019 and winter 2019–2020. Simulations of the NO2 tropospheric vertical column densities and surface concentrations from the Long-Term Ozone Simulation–European Operational Smog (LOTOS-EUROS) chemical transport model are also applied in the methodology. More than two hundred in situ air quality monitoring stations, reporting to the European Environment Agency (EEA) air quality database, are used to carry out comparisons with the model simulations and the spaceborne inferred surface concentrations. Stations are separated into seven types (urban traffic, suburban traffic, urban background, suburban background, rural background, suburban industrial and rural industrial) in order to examine the strengths and shortcomings of the different air quality markers, namely the NO2 vertical column densities and NO2 surface concentrations. S5P/TROPOMI NO2 surface concentrations are inferred by multiplying the fraction of the satellite and model NO2 vertical column densities with the model surface concentrations. The estimated inferred TROPOMI NO2 surface concentrations are examined further with the altering of three influencing factors: the model vertical leveling scheme, the versions of the TROPOMI NO2 data and the air mass factors applied to the satellite and model NO2 vertical column densities. Overall, the inferred TROPOMI NO2 surface concentrations show a better correlation with the in situ measurements for both time periods and all station types, especially for the industrial stations (R > 0.6) in winter. The calculated correlation for background stations is moderate for both periods (R~0.5 in summer and R > 0.5 in winter), whereas for traffic stations it improves in the winter (from 0.20 to 0.50). After the implementation of the air mass factors from the local model, the bias is significantly reduced for most of the station types, especially in winter for the background stations, ranging from +0.49% for the urban background to +10.37% for the rural background stations. The mean relative bias in winter between the inferred S5P/TROPOMI NO2 surface concentrations and the ground-based measurements for industrial stations is about −15%, whereas for traffic urban stations it is approximately −25%. In summer, biases are generally higher for all station types, especially for the traffic stations (~−75%), ranging from −54% to −30% for the background and industrial stations. [ABSTRACT FROM AUTHOR]

With the explosive growth of atmospheric data, machine learning models have achieved great success in air pollution forecasting because of their higher computational efficiency than the traditional chemical transport models. However, in previous studies, new prediction algorithms have been tested only at stations or in a small region; a large-scale air quality forecasting model remains lacking to date. Huge dimensionality also means that redundant input data may lead to increased complexity and therefore the over-fitting of machine learning models. Feature selection is a key topic in machine learning development, but it has not yet been explored in atmosphere-related applications. In this work, a regional feature selection-based machine learning (RFSML) system was developed, which is capable of predicting air quality in the short-term with high accuracy at the national scale. Ensemble-Shapley additive global importance analysis is combined with the RFSML system to extract significant regional features and eliminate redundant variables at an affordable computational expense. The significance of the regional features is also explained physically. Compared with a standard machine learning system fed with relative features, the RFSML system driven by the selected key features results in superior interpretability, less training time, and more accurate predictions. This study also provides insights into the difference in interpretability among machine learning models (i.e., random forest, gradient boosting, and multi-layer perceptron models). [ABSTRACT FROM AUTHOR]

Monitoring the spatial distribution and trends in surface greenhouse gas (GHG) fluxes, as well as flux attribution to natural and anthropogenic processes, is essential to track progress under the Paris Agreement and to inform its Global Stocktake. This study updates earlier syntheses (Petrescu et al., 2020, 2021, 2023) and provides a consolidated synthesis of CH4 emissions using bottom-up (BU) and top-down (TD) approaches for the European Union (EU) and seven additional countries with large anthropogenic and/or natural emissions (USA, Brazil, China, India, Indonesia, Russia, and the Democratic Republic of Congo (DR Congo)). The work utilizes updated National GHG Inventories (NGHGIs) reported by Annex I Parties under the United Nations Framework Convention on Climate Change (UNFCCC) in 2023 and the latest available Biennial Update Reports (BURs) reported by non-Annex I Parties. The NGHGIs are considered in an integrated analysis that also relies on independent flux estimates from global inventory datasets, process-based models, inverse modeling and, when available, respective uncertainties. Whenever possible, it extends the period to 2021. Comparing NGHGIs with other approaches reveals that differences in the emission sources that are included in the estimate is a key source of divergence between approaches. A key system boundary difference is whether both anthropogenic and natural fluxes are included and, if they are, how fluxes belonging to these two sources are grouped/partitioned. Additionally, the natural fluxes are sensitive to the prior geospatial distribution of emissions in atmospheric inversions. Over the studied period, the total CH4 emissions in the EU, USA, and Russia show a steady decreasing trend since 1990, while for the non-EU emitters analyzed in this study, Brazil, China, India, Indonesia, and DR Congo, CH4 emissions have generally increased. In the EU, the anthropogenic BU approaches are reporting relatively similar mean emissions over 2015 to 2020 of 18.5 ± 2.7 Tg CH4 yr-1 for EDGAR v7.0, 16 Tg CH4 yr-1 for GAINS and 19 Tg CH4 yr-1 for FAOSTAT, with the NGHGI estimates of 15 ± 1.8 Tg CH4 yr-1. Inversions give higher emission estimates as they include natural emissions. Over the same period, the three high-resolution regional inversions report a mean emission of 21 (19-25) Tg CH4 yr-1, while the mean of six coarser-resolution global inversions results in emission estimates of 24 (23-25) Tg CH4 yr-1. The magnitude of BU natural emissions (peatland and mineral soils, lakes and reservoirs, geological and biomass burning) accounts for 6.6 Tg CH4 yr-1 (Petrescu et al., 2023a) and explains the differences between the TD inversions and the BU estimates of anthropogenic emissions (including NGHGIs). For the other Annex I Parties in this study (USA and Russia), over 2015 to 2020, the mean of the four anthropogenic BU approaches reports 18.5 (13-27.9) Tg CH4 yr-1 for Russia and 29.1 (23.5- Tg CH4 yr-1 for the USA, against total TD mean estimates of 37 (30-43) Tg CH4 yr-1 and 43.4 (42-48) Tg CH4 yr-1, respectively. The averaged BU and TD natural emissions account for 16.2 Tg CH4 yr-1 for Russia and 14.6 Tg CH4 yr-1 for the USA, partly explaining the gap between the BU anthropogenic and total TD emissions. For the non-Annex I Parties, anthropogenic CH4 estimates from UNFCCC BURs show large differences with the other global inventory-based estimates and even more with atmospheric-based ones. This poses an important potential challenge to monitoring the progress of the global CH4 pledge and the Global Stocktake, not only from the availability of data but also its accuracy. By systematically comparing the BU with TD methods, this study provides recommendations for more robust comparisons of available data sources and hopes to steadily engage more Parties in using observational methods to complement their UNFCCC inventories, as well as considering their natural emissions. With anticipated improvements in atmospheric modeling and observations, as well as modeling of natural fluxes, future development needs to resolve knowledge gaps in both BU and TD approaches and to better quantify remaining uncertainty. Consequently, TD methods may emerge as a powerful tool for verifying emission inventories for CH4, and other GHGs and informing international climate policy. The referenced datasets related to figures are available at https://doi.org/10.5281/zenodo.10276087 (Petrescu et al., 2023b). [ABSTRACT FROM AUTHOR]

Super dust storms re-occurred over East Asia in 2021 spring and casted great health damages and property losses. It is essential to achieve an accurate dust forecast to reduce the damage for early warning. The forecasting system fundamentally relies on a numerical model which can forecast the full evolution of dust storms. However, large uncertainties exist in model forecasts. Meanwhile, various near-real-time observations are available that contain valuable dust information. A dust storm forecasting system is here developed through coupling a chemical transport model, LOTOS-EUROS, and Localized EnKF (LEnKF) assimilation approach. The assimilations are carried out via an interface of our self-designed assimilation toolbox, PyFilter v1.0. Ground-based PM 10 measurements from air quality monitoring network are assimilated. Sequential assimilation tests are carried out over the 2021 spring super dust storms. The results show that the assimilation-based forecasting system produces a promising dust forecast than model-only forecast, and the improvements is also validated through comparing to the independent MODIS aerosol optical depth (AOD). Superior performance is obtained when LEnKF is implemented, as the localization helps EnKF in resolving the PM 10 measurements that have a large spatial variability with limited ensemble members. In addition, sensitivity experiments are conducted to exploit the distance-dependent localization for the LEnKF. Considering both cases, the optimal choice of the distance is tested to be around 500 km: the larger distance is less effective in removing the spurious correction, while the smaller one easily falls into the local optimum and the model would become divergent rapidly. • A dust storm forecasting system is developed by coupling LOTOS-EUROS and EnKF. • Dust forecast is improved when data assimilation is applied. • LEnKF is proved to be superior than EnKF in dust storm forecasting. • Sensitivities of dust forecast to the localization distance in LEnKF are exploited. [ABSTRACT FROM AUTHOR]

This study investigates atmospheric δ 13 CH 4 trends, as produced by a global atmospheric transport model using CH 4 inversions from CarbonTracker-Europe CH 4 for 2000–2020, and compares them to observations. The CH 4 inversions include the grouping of the emissions both by δ 13 CH 4 isotopic signatures and process type to investigate the effect, and to estimate the CH 4 magnitudes and model CH 4 and δ 13 CH 4 trends. In addition to inversion results, simulations of the global atmospheric transport model were performed with modified emissions. The estimated global CH 4 trends for oil and gas were found to increase more than coal compared to the priors from 2000–2006 to 2007–2020. Estimated trends for coal emissions at 30 ∘ N–60 ∘ N are less than 50% of those from priors. Estimated global CH 4 rice emissions trends are opposite to priors, with the largest contribution from the EQ to 60 ∘ N. The results of this study indicate that optimizing wetland emissions separately produces better agreement with the observed δ 13 CH 4 trend than optimizing all biogenic emissions simultaneously. This study recommends optimizing separately biogenic emissions with similar isotopic signature to wetland emissions. In addition, this study suggests that fossil-based emissions were overestimated by 9% after 2012 and biogenic emissions are underestimated by 8% in the inversion using EDGAR v6.0 as priors. [ABSTRACT FROM AUTHOR]

Chemical transport models (CTM) are crucial for simulating the distribution of air pollutants, such as particulate matter, and evaluating their impact on the environment and human health. However, these models rely heavily on accurate emission inventory and meteorological inputs, usually obtained from reanalyzed weather data, such as the European Centre for Medium-Range Weather Forecasts (ECMWF). These inputs do not accurately reflect the complex topography and micro-scale meteorology in tropical regions where air pollution can pose a severe public health threat. We propose coupling the LOTOS–EUROS CTM model and the weather research and forecasting (WRF) model to improve LOTOS–EUROS representation. Using WRF as a meteorological driver provides high-resolution inputs for accurate pollutant simulation. We compared LOTOS–EUROS results when WRF and ECMWF provided the meteorological inputs during low and high pollutant concentration periods. The findings indicate that the WRF–LOTOS–EUROS coupling offers a more precise representation of the meteorology and pollutant dispersion than the default input of ECMWF. The simulations also capture the spatio-temporal variability of pollutant concentration and emphasize the importance of accounting for micro-scale meteorology and topography in air pollution modelling. [ABSTRACT FROM AUTHOR]

The chemical transport model LOTOS‐EUROS uses a volatility basis set (VBS) approach to represent the formation of secondary organic aerosol (SOA) in the atmosphere. Inclusion of the VBS approximately doubles the dimensionality of LOTOS‐EUROS and slows computation of the advection operator by a factor of two. This complexity limits SOA representation in operational forecasts. We develop a mass‐conserving dimensionality reduction method based on matrix factorization to find latent patterns in the VBS tracers that correspond to a smaller set of superspecies. Tracers are reversibly compressed to superspecies before transport, and the superspecies are subsequently decompressed to tracers for process‐based SOA modeling. This physically interpretable data‐driven method conserves the total concentration and phase of the tracers throughout the process. The superspecies approach is implemented in LOTOS‐EUROS and found to accelerate the advection operator by a factor of 1.5–1.8. Concentrations remain numerically stable over model simulation times of 2 weeks, including simulations at higher spatial resolutions than the data‐driven models were trained on. The reversible compression of VBS tracers enables detailed, process‐based SOA representation in LOTOS‐EUROS operational forecasts in a computationally efficient manner. Beyond this case study, the physically consistent data‐driven approach developed in this work enforces conservation laws that are essential to other Earth system modeling applications, and generalizes to other processes where computational benefit can be gained from a two‐way mapping between detailed process variables and their representation in a reduced‐dimensional space. Plain Language Summary: The chemical composition of the atmosphere is a complex system involving many physical processes. Computer models can be used to improve our understanding of how these processes interact, as well as simulate hypothetical scenarios to support scientifically‐informed climate and air quality policies. However, complicated models with many variables can take a lot of time to run. The LOTOS‐EUROS model spends a large fraction of time and computational resources on simulating the transport of chemical species, like particulate matter, by wind. We combine data‐driven approaches with domain knowledge to reduce the number of variables while ensuring essential properties are conserved: we model representative combinations of chemical species that are transported all at once, rather than transport each species individually. This leads to faster and cheaper simulations without loss of scientific detail or internal consistency. Key Points: We develop a data‐driven method to find a reduced‐dimension set of superspecies representing tracers in a chemical transport modelThis method is designed to be physically consistent, preserving information on phase and conserving mass to machine precisionAdvecting the superspecies accelerates the advection operator by a factor of 1.5–1.8 [ABSTRACT FROM AUTHOR]

This study investigates the contribution of different CH4 sources to the seasonal cycle of δ 13 C during 2000–2012 by using the TM5 atmospheric transport model, including spatially varying information on isotopic signatures. The TM5 model is able to produce the background seasonality of δ 13 C, but the discrepancies compared to the observations arise from incomplete representation of the emissions and their source-specific signatures. Seasonal cycles of δ 13 C are found to be an inverse of CH4 cycles in general, but the anti-correlations between CH4 and δ 13 C are imperfect and experience a large variation ( p = −0.35 to −0.91) north of 30° S. We found that wetland emissions are an important driver in the δ 13 C seasonal cycle in the Northern Hemisphere and Tropics, and in the Southern Hemisphere Tropics, emissions from fires contribute to the enrichment of δ 13 C in July–October. The comparisons to the observations from 18 stations globally showed that the seasonal cycle of EFMM emissions in the EDGAR v5.0 inventory is more realistic than in v4.3.2. At northern stations (north of 55° N), modeled δ 13 C amplitudes are generally smaller by 12–68%, mainly because the model could not reproduce the strong depletion in autumn. This indicates that the CH4 emission magnitude and seasonal cycle of wetlands may need to be revised. In addition, results from stations in northern latitudes (19–40° N) indicate that the proportion of biogenic to fossil-based emissions may need to be revised, such that a larger portion of fossil-based emissions is needed during summer. [ABSTRACT FROM AUTHOR]

Two different data assimilation techniques have been applied to assess exceedances of the daily and annual mean limit values for PM10 on the regional scale in Europe. The two methods include a statistical interpolation method (SI), based on residual kriging after linear regression of the model, and Ensemble Kalman filtering (EnKF). Both methods are applied using the LOTOS-EUROS model. Observations for the assimilation and validation of the methods have been retrieved from the Airbase database using rural background stations only. For the period studied, 2003, 127 suitable stations were available. The LOTOS-EUROS model is found to underestimate PM10 concentrations by a factor of 2. This large model bias is found to be prohibitive for the effective use of the EnKF methodology and a bias correction was required for the filter to function effectively. The results of the study show that both methods provide significant improvement on the model calculations when compared to an independent set of validation stations. The total root mean square error of the daily mean concentrations of PM10 at the validation stations was reduced from 16.7μgm−3 for the model to 9.2μgm−3 using SI and to 13.5μgm−3 using EnKF. Similarly, correlation (R 2) is also significantly improved from 0.21 for the model to 0.66 using SI and 0.41 using EnKF. Significant improvement in the annual mean and number of exceedance days of PM10 is also seen. In addition to the validation of the methods, maps of exceedances and their associated uncertainty are presented. The most effective methodology is found to be the statistical interpolation method. The application of EnKF is novel and yields promising results, although its application to PM10 still needs to be improved. [Copyright &y& Elsevier]

This study aims at estimating errors to be accounted for in atmospheric inversions of methane (CH4) emissions at the European scale. Four types of errors are estimated in the concentration space over the model domain and at selected measurement sites. Furthermore, errors in emission inventories are estimated at country and source sector scales. A technically ready method is used, which is implemented by running a set of simulations of hourly CH4 mixing ratios for 2015 using two area-limited transport models at three horizontal resolutions with multiple data sets of emissions and boundary and initial conditions as inputs. The obtained error estimates provide insights into how these errors could be treated in an inverse modelling system for inverting CH4 emissions over Europe. The main results show that sources of transport errors may better be controlled alongside the emissions, which differs from usual inversion practices. The average total concentration error is estimated at 29 ppb. The assessed error of total CH4 emissions is 22% and emission errors are heterogeneous at sector (23-49%) and country scales (16-124%), with largest errors occurring in the waste sector due to uncertainties in activity data and emission factors and in Finland due to uncertainties in natural wetland emissions. [ABSTRACT FROM AUTHOR]

In this paper, we propose an efficient and practical implementation of the ensemble Kalman filter via shrinkage covariance matrix estimation. Our filter implementation combines information brought by an ensemble of model realizations, and that based on our prior knowledge about the dynamical system of interest. We perform the combination of both sources of information via optimal shrinkage factors. The method exploits the rank-deficiency of ensemble covariance matrices to provide an efficient and practical implementation of the analysis step in EnKF based formulations. Localization and inflation aspects are discussed, as well. Experimental tests are performed to assess the accuracy of our proposed filter implementation by employing an Advection Diffusion Model and an Atmospheric General Circulation Model. The experimental results reveal that the use of our proposed filter implementation can mitigate the impact of sampling noise, and even more, it can avoid the impact of spurious correlations during assimilation steps. [ABSTRACT FROM AUTHOR]

In previous studies, a number of model-based dust forecasts and early warning systems have been developed for the prevention of environmental impacts due to dusts. However, the accuracy of the model is limited by imperfect identification of dust emissions, in particular by the friction velocity threshold parameterization in the emission process. In this study, an integrated dust storm forecast system - LOTOS-EUROS/Dust coupled with reduced-tangent-linearization 4DVar data assimilation has been developed. In order to overcome the inflexibility and inaccuracy of the existing friction velocity threshold parameterization in large-scale models, a spatially varying multiplicative factor for the threshold is introduced. This parameter is estimated by assimilating measurements from a field station network developed by China Ministry of Environmental Protection. The data assimilation algorithm is adjoint-free, and its computational complexity increases with the number of uncertain parameters. Two model reducing techniques, sensitivity-based parameter filters and proper orthogonal decomposition, are sequentially implemented after each other, which lead to a reduction of parameter dimension from initially O ( 10 4 ) to O ( 10 2 ) . Twin experiments are conducted to evaluate the impact of assimilation settings on the dust forecast accuracy. In addition, experiments with real observations are conducted. However, these observations also reflect the aerosol concentration from local emissions. To effectively use these observations as representative for dust concentrations, an observation bias correction and a variable representation error are designed. Improvements on the dust storm forecast with our system are demonstrated. [ABSTRACT FROM AUTHOR]