Interregional Air Pollutant Transport: The Linearity Question

This report contains extended abstracts from an international meeting held in Budapest, Hungary. Its main subject is the question of proportionality and linearity between emissions and deposition/airborne concentration of air pollutants including sulfur, nitrogen, oxidants, and acidity. Session topics (which serve here as section headings) included analysis of measurements, ammonia and its implications for linearity, modeling with emphasis on chemistry, simplified approaches to the linearity issue, and results from long-range transport models. Linearity was found to be strongly dependent on the distance between emitters and receptors, the averaging time of pollutants, and the form of deposition

Retrieval methods of effective cloud cover from the GOME instrument: an intercomparison

The radiative scattering by clouds leads to errors in the retrieval of column densities and concentration profiles of atmospheric trace gas species from satellites. Moreover, the presence of clouds changes the UV actinic flux and the photo-dissociation rates of various species significantly. The Global Ozone Monitoring Experiment (GOME) instrument on the ERS-2 satellite, principally designed to retrieve trace gases in the atmosphere, is also capable of detecting clouds. Four cloud fraction retrieval methods for GOME data that have been developed are discussed in this paper (the Initial Cloud Fitting Algorithm, the PMD Cloud Recognition Algorithm, the Optical Cloud Recognition Algorithm (an in-house version and the official implementation) and the Fast Retrieval Scheme for Clouds from the Oxygen A-band). Their results of cloud fraction retrieval are compared to each-other and also to synoptic surface observations. It is shown that all studied retrieval methods calculate an effective cloud fraction that is related to a cloud with a high optical thickness. Generally, we found ICFA to produce the lowest cloud fractions, followed by our in-house OCRA implementation, FRESCO, PC2K and finally the official OCRA implementation along four processed tracks (+2%, +10%, +15% and +25% compared to ICFA respectively). Synoptical surface observations gave the highest absolute cloud fraction when compared with individual PMD sub-pixels of roughly the same size

Retrieval methods of effective cloud cover for the GOME instrument: an intercomparison

International audienceThe radiative scattering by clouds leads to errors in the retrieval of column densities and concentration profiles of atmospheric trace gas species from satellites. Moreover, the presence of clouds changes the UV actinic flux and the photo-dissociation rates of various species significantly. The Global Ozone Monitoring Experiment (GOME) instrument on the ERS-2 satellite, principally designed to retrieve trace gases in the atmosphere is also capable of detecting clouds. Four cloud fraction retrieval methods for GOME data that have been developed are discussed in this paper (the Initial Cloud Fitting Algorithm, the PMD Cloud Retrieval Algorithm, the Optical Cloud Recognition Algorithm and the Fast Retrieval Scheme for Cloud Observables). Their results of cloud fraction retrieval are compared to each-other and also to synoptic surface observations. It is shown that all studied retrieval methods calculate an effective cloud fraction that is related to a cloud with a high optical thickness. Generally, we found ICFA to produce the lowest cloud fractions, followed by OCRA, then FRESCO and PC2K along four processed tracks (+2%, +10% and +15% compared to ICFA respectively). Synoptical surface observations gave the highest absolute cloud fraction when compared with individual PMD sub-pixels of roughly the same size

The nitrate aerosol field over Europe: simulations with an atmospheric chemistry-transport model of intermediate complexity

International audienceNitrate is an important component of fine aerosols in Europe. We present a model simulation for the year 1995 in which we account for the formation of the ammonium nitrate, a semi volatile component. For this purpose, LOTOS, a chemistry-transport model of intermediate complexity, was extended with a thermodynamic equilibrium module and additional relevant processes to account for aerosol formation and deposition. Our earlier analysis of data on (ammonium) nitrate in Europe was used for model evaluation. During winter, fall and especially spring high nitrate levels are projected over north western, central and eastern Europe. During winter nitrate concentrations are highest in the Po valley, Italy. This is in accordance with the field that was constructed from the data. In winter nitric acid, the precursor for aerosol nitrate, is formed through heterogeneous reactions on the surface of aerosols. Appreciable ammonium nitrate concentrations in summer are limited to those areas with high ammonia emissions, e.g. The Netherlands, since high ammonia concentrations are necessary to stabilise this aerosol component at high temperatures. Averaged over all stations the model reproduces the measured concentrations for NO3, SO4, NH4, TNO3, TNH4 and SO2 within 20%. The daily variation is captured well, albeit that the model does not always represents the amplitude of single events. The model underestimates wet deposition which was attributed to the crude representation of cloud processes. The treatment of ammonia was found to be the major source for uncertainties in the model representation of secondary aerosols. Also, inclusion of sea salt is necessary to properly assess the nitrate and nitric acid levels in marine areas. Over Europe the annual forcing by nitrate is calculated to be 25% of that by sulphate. In summer nitrate is found to be regionally important, e.g. in The Netherlands, where the forcing of nitrate and sulphate are calculated to be equal. In winter, spring and fall the nitrate forcing over Europe is about half that by sulphate. Over north western Europe and the alpine region the forcing by nitrate was calculated to be similar to that of sulphate. Overall, nitrate forcing is significant and should be taken into account to estimate the impact of regional climate change in Europe

Secondary inorganic aerosol simulations for Europe with special attention to nitrate

International audienceNitrate is an important component of (secondary inorganic) fine aerosols in Europe. We present a model simulation for the year 1995 in which we account for the formation of secondary inorganic aerosols including ammonium sulphate and ammonium nitrate, a semi volatile component. For this purpose, the chemistry-transport model LOTOS was extended with a thermodynamic equilibrium module and additional relevant processes to account for secondary aerosol formation and deposition. During winter, fall and especially spring high nitrate levels are projected over north western, central and eastern Europe. During winter nitrate concentrations are highest in Italy, in accordance with observed data. In winter nitric acid, the precursor for aerosol nitrate is formed through heterogeneous reactions on the surface of aerosols. Modelled and observed sulphate concentrations show little seasonal variation. Compared to sulphate levels, appreciable ammonium nitrate concentrations in summer are limited to those areas with high ammonia emissions, e.g. the Netherlands, since high ammonia concentrations are necessary to stabilise this aerosol component at high temperatures. As a consequence of the strong seasonal variation in nitrate levels the AOD depth of nitrate over Europe is especially significant compared to that of sulphate in winter and spring when equal AOD values are calculated over large parts of Europe. Averaged over all stations the model reproduces the measured concentrations for NO3, SO4, NH4, TNO3 (HNO3+NO3), TNH4 (NH3+NH4) and SO2 within 20%. The daily variation is captured well, albeit that the model does not always represent the amplitude of single events. The model underestimates wet deposition which was attributed to the crude representation of cloud processes. Comparison of retrieved and computed aerosol optical depth (AOD) showed that the model underestimates AOD significantly, which was expected due to the lack of carbonaceous aerosols, sea salt and dust in the model. The treatment of ammonia was found to be a major source for uncertainties in the model representation of secondary aerosols. Also, inclusion of sea salt is necessary to properly assess the nitrate and nitric acid levels in marine areas

Spatial variation of aerosol properties over Europe derived from satellite observations and comparison with model calculations

International audienceAerosol optical depths (AOD) and Angström coefficients over Europe were retrieved using data from the ATSR-2 radiometer on board the ESA satellite ERS-2, for August 1997. Taking advantage of the nadir and forward view of the ATSR-2, the dual view algorithm was used over land to eliminate the influence of the surface reflection. Over sea the AOD was retrieved using only the forward observations. Retrieved aerosol optical properties are in good agreement with those from ground-based sunphotometers. The AOD and Angström coefficients together yield information on the column integrated effective aerosol distribution. Observed regional variations of the AOD and Angström coefficient are related to anthropogenic emissions of aerosol precursors such as SO2 and NOx in the major European industrial and urban areas, and their subsequent transformation into the aerosol phase. The influence of anthropogenic aerosols such as ammonium sulphate and ammonium nitrate on the total AOD is estimated using a regional chemistry transport model. Sulphate is estimated to contribute from 15% in very clean areas to 70% in polluted areas, the contribution of nitrate is between 5% and 25% over most of Europe. This paper shows the great importance of nitrate in summer over The Netherlands

Spatial variation of aerosol properties derived from satellite observations

International audienceAerosol optical depths (AOD) and Angström coefficients over Europe were retrieved using data from the ATSR-2 radiometer on board the ESA satellite ERS-2, for August 1997. Taking advantage of the nadir and forward view of the ATSR-2, the dual view algorithm was used over land to eliminate the influence of the surface reflection. Over sea the AOD was retrieved using only the forward observations. Retrieved aerosol optical properties are in good agreement with those from ground-based sunphotometers. The AOD and Angström coefficients together yield information on the column integrated effective aerosol distribution. Observed regional variations of the AOD and Angström coefficient are related to anthropogenic emissions of aerosol precursors such as SO2 and NOx in the major European industrial and urban areas, and their subsequent transformation into the aerosol phase. The influence of anthropogenic aerosols such as ammonium sulphate and ammonium nitrate on the total AOD is estimated using a regional chemistry transport model. Sulphate is estimated to contribute from 15% in very clean areas to 70% in polluted areas, the contribution of nitrate is between 5% and 25% over most of Europe. This paper shows the great importance of nitrate in summer over The Netherlands

Combining data from the distributed GRUAN site Lauder–Invercargill, New Zealand, to provide a site atmospheric state best estimate of temperature

A site atmospheric state best estimate (SASBE) of the temperature profile above the GCOS (Global Climate Observing System) Reference Upper-Air Network (GRUAN) site at Lauder, New Zealand, has been developed. Data from multiple sources are combined within the SASBE to generate a high temporal resolution data set that includes an estimate of the uncertainty on every value.The SASBE has been developed to enhance the value of measurements made at the distributed GRUAN site at Lauder and Invercargill (about 180&thinsp;km apart), and to demonstrate a methodology which can be adapted to other distributed sites. Within GRUAN, a distributed site consists of a cluster of instruments at different locations.The temperature SASBE combines measurements from radiosondes and automatic weather stations at Lauder and Invercargill, and ERA5 reanalysis, which is used to calculate a diurnal temperature cycle to which the SASBE converges in the absence of any measurements.The SASBE provides hourly temperature profiles at 16 pressure levels between the surface and 10&thinsp;hPa for the years 1997 to 2012. Every temperature value has an associated uncertainty which is calculated by propagating the measurement uncertainties, the ERA5 ensemble standard deviations, and the ERA5 representativeness uncertainty through the retrieval chain. The SASBE has been long-term archived and is identified using the digital object identifier https://doi.org/10.5281/zenodo.1195779.The study demonstrates a method to combine data collected at distributed sites. The resulting best-estimate temperature data product for Lauder is expected to be valuable for satellite and model validation as measurements of atmospheric essential climate variables are sparse in the Southern Hemisphere. The SASBE could, for example, be used to constrain a radiative transfer model to provide top-of-the-atmosphere radiances with traceable uncertainty estimates.</p

Curriculum vitae of the LOTOS-EUROS (v2.0) chemistry transport model

The development and application of chemistry transport models has a long tradition. Within the Netherlands the LOTOS–EUROS model has been developed by a consortium of institutes, after combining its independently developed predecessors in 2005. Recently, version 2.0 of the model was released as an open-source version. This paper presents the curriculum vitae of the model system, describing the model's history, model philosophy, basic features and a validation with EMEP stations for the new benchmark year 2012, and presents cases with the model's most recent and key developments. By setting the model developments in context and providing an outlook for directions for further development, the paper goes beyond the common model description. With an origin in ozone and sulfur modelling for the models LOTOS and EUROS, the application areas were gradually extended with persistent organic pollutants, reactive nitrogen, and primary and secondary particulate matter. After the combination of the models to LOTOS–EUROS in 2005, the model was further developed to include new source parametrizations (e.g. road resuspension, desert dust, wildfires), applied for operational smog forecasts in the Netherlands and Europe, and has been used for emission scenarios, source apportionment, and long-term hindcast and climate change scenarios. LOTOS–EUROS has been a front-runner in data assimilation of ground-based and satellite observations and has participated in many model intercomparison studies. The model is no longer confined to applications over Europe but is also applied to other regions of the world, e.g. China. The increasing interaction with emission experts has also contributed to the improvement of the model's performance. The philosophy for model development has always been to use knowledge that is state of the art and proven, to keep a good balance in the level of detail of process description and accuracy of input and output, and to keep a good record on the effect of model changes using benchmarking and validation. The performance of v2.0 with respect to EMEP observations is good, with spatial correlations around 0.8 or higher for concentrations and wet deposition. Temporal correlations are around 0.5 or higher. Recent innovative applications include source apportionment and data assimilation, particle number modelling, and energy transition scenarios including corresponding land use changes as well as Saharan dust forecasting. Future developments would enable more flexibility with respect to model horizontal and vertical resolution and further detailing of model input data. This includes the use of different sources of land use characterization (roughness length and vegetation), detailing of emissions in space and time, and efficient coupling to meteorology from different meteorological models

Curriculum vitae of the LOTOS–EUROS (v2.0) chemistry transport model

The development and application of chemistry transport models has a long tradition. Within the Netherlands the LOTOS–EUROS model has been developed by a consortium of institutes, after combining its independently developed predecessors in 2005. Recently, version 2.0 of the model was released as an open-source version. This paper presents the curriculum vitae of the model system, describing the model's history, model philosophy, basic features and a validation with EMEP stations for the new benchmark year 2012, and presents cases with the model's most recent and key developments. By setting the model developments in context and providing an outlook for directions for further development, the paper goes beyond the common model description. With an origin in ozone and sulfur modelling for the models LOTOS and EUROS, the application areas were gradually extended with persistent organic pollutants, reactive nitrogen, and primary and secondary particulate matter. After the combination of the models to LOTOS–EUROS in 2005, the model was further developed to include new source parametrizations (e.g. road resuspension, desert dust, wildfires), applied for operational smog forecasts in the Netherlands and Europe, and has been used for emission scenarios, source apportionment, and long-term hindcast and climate change scenarios. LOTOS–EUROS has been a front-runner in data assimilation of ground-based and satellite observations and has participated in many model intercomparison studies. The model is no longer confined to applications over Europe but is also applied to other regions of the world, e.g. China. The increasing interaction with emission experts has also contributed to the improvement of the model's performance. The philosophy for model development has always been to use knowledge that is state of the art and proven, to keep a good balance in the level of detail of process description and accuracy of input and output, and to keep a good record on the effect of model changes using benchmarking and validation. The performance of v2.0 with respect to EMEP observations is good, with spatial correlations around 0.8 or higher for concentrations and wet deposition. Temporal correlations are around 0.5 or higher. Recent innovative applications include source apportionment and data assimilation, particle number modelling, and energy transition scenarios including corresponding land use changes as well as Saharan dust forecasting. Future developments would enable more flexibility with respect to model horizontal and vertical resolution and further detailing of model input data. This includes the use of different sources of land use characterization (roughness length and vegetation), detailing of emissions in space and time, and efficient coupling to meteorology from different meteorological models