Modelling the chemically aged and mixed aerosols over the eastern central Atlantic Ocean – potential impacts

Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size distribution, using chemistry-transport models, satellite data and in situ measurements. We focus on August 2005, a period with intense hurricane and tropical storm activity over the Atlantic Ocean. A mixture of anthropogenic (sulphates, nitrates), natural (desert dust, sea salt) and chemically aged (sulphate and nitrate on dust) aerosols is found entering the hurricane genesis region, most likely interacting with clouds in the area. Results from our modelling study suggest rather small amounts of accumulation mode desert dust, sea salt and chemically aged dust aerosols in this Atlantic Ocean region. Aerosols of smaller size (Aitken mode) are more abundant in the area and in some occasions sulphates of anthropogenic origin and desert dust are of the same magnitude in terms of number concentrations. Typical aerosol number concentrations are derived for the vertical layers near shallow cloud formation regimes, indicating that the aerosol number concentration can reach several thousand particles per cubic centimetre. The vertical distribution of the aerosols shows that the desert dust particles are often transported near the top of the marine cloud layer as they enter into the region where deep convection is initiated. The anthropogenic sulphate aerosol can be transported within a thick layer and enter the cloud deck through multiple ways (from the top, the base of the cloud, and by entrainment). The sodium (sea salt related) aerosol is mostly found below the cloud base. The results of this work may provide insights relevant for studies that consider aerosol influences on cloud processes and storm development in the Central Atlantic region

Methane and ethane emission scenarios for potential shale gas production in Europe

A main concern surrounding (shale) gas production and exploitation is the leakage of methane, a potent greenhouse gas. High leakage rates have been observed outside of Europe but the representativeness of these observations for Europe is unknown. To facilitate the monitoring of methane leakage from a future shale gas industry in Europe we developed potential production scenarios for ten major shale gas plays and identified a suitable tracer in (shale) gas to distinguish oil and gas related emissions from other methane sources. To distinguish gas leakage from other methane sources we propose ethane, a known tracer for leakage from oil and gas production but absent in emissions from other important methane sources in Europe. Ethane contents for the ten plays are estimated from a European gas composition database and shale gas composition and reservoir data from the US, resulting in three different classes of ethane to methane ratios in the raw gas (0.015, 0.04 and 0.1). The ethane content classes have a relation with the average thermal maturity, a basic shale gas reservoir characteristic, which is known for all ten European shale gas plays. By assuming different production scenarios in addition to a range of possible gas leakage rates, we estimate potential ethane tracer release by shale gas play. Ethane emissions are estimated by play following a low, medium or high gas production scenario in combination with leakage rates ranging from 0.2&thinsp;%–10&thinsp;% based on observed leakage rates in the US.</p

Intercomparison of detection and quantification methods for methane emissions from the natural gas distribution network in Hamburg, Germany

In August and September 2020, three different measurement methods for quantifying methane (CH4) emissions from leaks in urban gas distribution networks were applied and compared in Hamburg, Germany: the “mobile”, “tracer release”, and “suction” methods. The mobile and tracer release methods determine emission rates to the atmosphere from measurements of CH4 mole fractions in the ambient air, and the tracer release method also includes measurement of a gaseous tracer. The suction method determines emission rates by pumping air out of the ground using soil probes that are placed above the suspected leak location. The quantitative intercomparison of the emission rates from the three methods at a small number of locations is challenging because of limitations of the different methods at different types of leak locations. The mobile method was designed to rapidly quantify the average or total emission rate of many gas leaks in a city, but it yields a large emission rate uncertainty for individual leak locations. Emission rates determined for individual leak locations with the tracer release technique are more precise because the simultaneous measurement of the tracer released at a known rate at the emission source eliminates many of the uncertainties encountered with the mobile method. Nevertheless, care must be taken to properly collocate the tracer release and the leak emission points to avoid biases in emission rate estimates. The suction method could not be completed or applied at locations with widespread subsurface CH4 accumulation or due to safety measures. While the number of gas leak locations in this study is small, we observe a correlation between leak emission rate and subsurface accumulation. Wide accumulation places leaks into a safety category that requires immediate repair so that the suction method cannot be applied to these larger leaks in routine operation. This introduces a sampling bias for the suction method in this study towards the low-emission leaks, which do not require immediate repair measures. Given that this study is based on random sampling, such a sampling bias may also exist for the suction method outside of this study. While an investigation of the causal relationship between safety category and leak size is beyond the scope of this study, on average higher emission rates were observed from all three measurement-based quantification methods for leaks with higher safety priority compared to the leaks with lower safety concern. The leak locations where the suction method could not be applied were the biggest emitters, as confirmed by the emission rate quantifications using mobile and tracer methods and an engineering method based on the leak's diameter, pipeline overpressure, and depth at which the pipeline is buried. The corresponding sampling bias for the suction technique led to a low bias in derived emission rates in this study. It is important that future studies using the suction method account for any leaks not quantifiable with this method in order to avoid biases, especially when used to inform emission inventories.</p

Evaluation of a three-dimensional chemical transport model (PMCAMx) in the European domain during the EUCAARI May 2008 campaign

PMCAMx-2008, a detailed three-dimensional chemical transport model (CTM), was applied to Europe to simulate the mass concentration and chemical composition of particulate matter (PM) during May 2008. The model includes a state-of-the-art organic aerosol module which is based on the volatility basis set framework treating both primary and secondary organic components as semivolatile and photochemically reactive. The model performance is evaluated against high time resolution aerosol mass spectrometer (AMS) ground and airborne measurements. Overall, organic aerosol is predicted to account for 32% of total PM&lt;sub&gt;1&lt;/sub&gt; at ground level during May 2008, followed by sulfate (30%), crustal material and sea-salt (14%), ammonium (13%), nitrate (7%), and elemental carbon (4%). The model predicts that fresh primary OA (POA) is a small contributor to organic PM concentrations in Europe during late spring, and that oxygenated species (oxidized primary and biogenic secondary) dominate the ambient OA. The Mediterranean region is the only area in Europe where sulfate concentrations are predicted to be much higher than the OA, while organic matter is predicted to be the dominant PM&lt;sub&gt;1&lt;/sub&gt; species in central and northern Europe. The comparison of the model predictions with the ground measurements in four measurement stations is encouraging. The model reproduces more than 94% of the daily averaged data and more than 87% of the hourly data within a factor of 2 for PM&lt;sub&gt;1&lt;/sub&gt; OA. The model tends to predict relatively flat diurnal profiles for PM&lt;sub&gt;1&lt;/sub&gt; OA in many areas, both rural and urban in agreement with the available measurements. The model performance against the high time resolution airborne measurements at multiple altitudes and locations is as good as its performance against the ground level hourly measurements. There is no evidence of missing sources of OA aloft over Europe during this period

Quantification of carbon monoxide emissions from African cities using TROPOMI

Carbon monoxide (CO) is an air pollutant that plays an important role in atmospheric chemistry and is mostly emitted by forest fires and incomplete combustion in, for example, road transport, residential heating, and industry. As CO is co-emitted with fossil fuel CO2 combustion emissions, it can be used as a proxy for CO2. Following the Paris Agreement, there is a need for independent verification of reported activity-based bottom-up CO2 emissions through atmospheric measurements. CO can be observed daily at a global scale with the TROPOspheric Monitoring Instrument (TROPOMI) satellite instrument with daily global coverage at a resolution down to 5.5 × 7 km2. To take advantage of this unique TROPOMI dataset, we develop a cross-sectional flux-based emission quantification method that can be applied to quantify emissions from a large number of cities, without relying on computationally expensive inversions. We focus on Africa as a region with quickly growing cities and large uncertainties in current emission estimates. We use a full year of high-resolution Weather Research and Forecasting (WRF) simulations over three cities to evaluate and optimize the performance of our cross-sectional flux emission quantification method and show its reliability down to emission rates of 0.1 Tg CO yr−1. Comparison of the TROPOMI-based emission estimates to the Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa (DACCIWA) and Emissions Database for Global Atmospheric Research (EDGAR) bottom-up inventories shows that CO emission rates in northern Africa are underestimated in EDGAR, suggesting overestimated combustion efficiencies. We see the opposite when comparing TROPOMI to the DACCIWA inventory in South Africa and Côte d'Ivoire, where CO emission factors appear to be overestimated. Over Lagos and Kano (Nigeria) we find that potential errors in the spatial disaggregation of national emissions cause errors in DACCIWA and EDGAR respectively. Finally, we show that our computationally efficient quantification method combined with the daily TROPOMI observations can identify a weekend effect in the road-transport-dominated CO emissions from Cairo and Algiers.</p

Impact of forest fires, biogenic emissions and high temperatures on the elevated Eastern Meditteranean ozone levels during the hot summer of 2007

The hot summer of 2007 in southeast Europe has been studied using two regional atmospheric chemistry models; WRF-Chem and EMEP MSC-W. The region was struck by three heat waves and a number of forest fire episodes, greatly affecting air pollution levels. We have focused on ozone and its precursors using state-of-the-art inventories for anthropogenic, biogenic and forest fire emissions. The models have been evaluated against measurement data, and processes leading to ozone formation have been quantified. Heat wave episodes are projected to occur more frequently in a future climate, and therefore this study also makes a contribution to climate change impact research. The plume from the Greek forest fires in August 2007 is clearly seen in satellite observations of CO and NO2 columns, showing extreme levels of CO in and downwind of the fires. Model simulations reflect the location and influence of the fires relatively well, but the modelled magnitude of CO in the plume core is too low. Most likely, this is caused by underestimation of CO in the emission inventories, suggesting that the CO/NOx ratios of fire emissions should be re-assessed. Moreover, higher maximum values are seen in WRF-Chem than in EMEP MSC-W, presumably due to differences in plume rise altitudes as the first model emits a larger fraction of the fire emissions in the lowermost model layer. The model results are also in fairly good agreement with surface ozone measurements. Biogenic VOC emissions reacting with anthropogenic NOx emissions are calculated to contribute significantly to the levels of ozone in the region, but the magnitude and geographical distribution depend strongly on the model and biogenic emission module used. During the July and August heat waves, ozone levels increased substantially due to a combination of forest fire emissions and the effect of high temperatures. We found that the largest temperature impact on ozone was through the temperature dependence of the biogenic emissions, closely followed by the effect of reduced dry deposition caused by closing of the plants’ stomata at very high temperatures. The impact of high temperatures on the ozone chemistry was much lower. The results suggest that forest fire emissions, and the temperature effect on biogenic emissions and dry deposition, will potentially lead to substantial ozone increases in a warmer climate

Towards an online-coupled chemistry-climate model: evaluation of trace gases and aerosols in COSMO-ART

Peer reviewe

Emissions of methane in Europe inferred by total column measurements

Using five long-running ground-based atmospheric observatories in Europe, we demonstrate the utility of long-term, stationary, ground-based measurements of atmospheric total columns for verifying annual methane emission inventories. Our results indicate that the methane emissions for the region in Europe between Orléans, Bremen, Białystok, and Garmisch-Partenkirchen are overestimated by the state-of-the-art inventories of the Emissions Database for Global Atmospheric Research (EDGAR) v4.2 FT2010 and the high-resolution emissions database developed by the Netherlands Organisation for Applied Scientific Research (TNO) as part of the Monitoring Atmospheric Composition and Climate project (TNO-MACC_III), possibly due to the disaggregation of emissions onto a spatial grid. Uncertainties in the carbon monoxide inventories used to compute the methane emissions contribute to the discrepancy between our inferred emissions and those from the inventories

Modelling the dispersion of particle numbers in five European cities

We present an overview of the modelling of particle number concentrations (PNCs) in five major European cities, namely Helsinki, Oslo, London, Rotterdam, and Athens, in 2008. Novel emission inventories of particle numbers have been compiled both on urban and European scales. We used atmospheric dispersion modelling for PNCs in the five target cities and on a European scale, and evaluated the predicted results against available measured concentrations. In all the target cities, the concentrations of particle numbers (PNs) were mostly influenced by the emissions originating from local vehicular traffic. The influence of shipping and harbours was also significant for Helsinki, Oslo, Rotterdam, and Athens, but not for London. The influence of the aviation emissions in Athens was also notable. The regional background concentrations were clearly lower than the contributions originating from urban sources in Helsinki, Oslo, and Athens. The regional background was also lower than urban contributions in traffic environments in London, but higher or approximately equal to urban contributions in Rotterdam. It was numerically evaluated that the influence of coagulation and dry deposition on the predicted PNCs was substantial for the urban background in Oslo. The predicted and measured annual average PNCs in four cities agreed within approximatelyPeer reviewe

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