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The Equilibrium Simplified Aerosol Model for Climate version 12 (EQSAM4Clim-v12) has recently been revised to provide an accurate and efficient method for calculating the acidity of atmospheric particles. EQSAM4Clim is based on an analytical concept that is not only sufficiently fast for chemical weather prediction applications but also free of numerical noise, which also makes it attractive for air quality forecasting. EQSAM4Clim allows the calculation of aerosol composition based on the gas–liquid–solid and the reduced gas–liquid partitioning with the associated water uptake for both cases and can therefore provide important information about the acidity of the aerosols. Here we provide a comprehensive description of the recent changes made to the aerosol acidity parameterization (referred to as a version 12) which builds on the original EQSAM4Clim. We evaluate the pH improvements using a detailed box model and compare them against previous model calculations and both ground-based and aircraft observations from the USA and China, covering different seasons and scenarios. We show that, in most cases, the simulated pH is within reasonable agreement with the reference results of the Extended Aerosol Inorganics Model (E-AIM) and of satisfactory accuracy. [ABSTRACT FROM AUTHOR]

The atmospheric composition forecasting system used to produce the CAMS forecasts of global aerosol and trace gases distributions, IFS-COMPO, undergoes periodic upgrades. In this paper we describe the development of the future operational cycle 49R1, and focus on the implementation of the thermodynamical model EQSAM4Clim version 12 for describing gas-aerosol partitioning processes for nitrate and ammonium and for providing diagnostic aerosol, cloud and precipitation pH values at global scale. This information on aerosol acidity influences tropospheric chemistry processes associated with aqueous phase chemistry and wet deposition. The other updates to cycle 49R1 include modifications to the description of Desert Dust, Sea-salt aerosols, Carbonaceous aerosols and the size description for the calculation of aerosol optics. The implementation of EQSAM4Clim significantly improves the partitioning of reactive nitrogen compounds decreasing surface concentrations of both nitrate and ammonium, which reduces PM2.5 biases for Europe, U.S. and China, especially during summertime. For aerosol optical depth there is generally a decrease in the simulated biases for wintertime, and for some regions an increase in the bias for summertime. Improvements in the simulated Ångström exponent is noted for almost all regions, resulting in generally a good agreement with observations. The diagnostic aerosol and precipitation pH calculated by EQSAM4Clim have been compared against results from previous simulations (for aerosol pH) and against ground observations (for precipitation pH), with the temporal distribution in the annual mean values showing good agreement against the regional observational datasets. The use of aerosol acidity only has a relatively smaller impact on the aqueous-phase production of sulphate when compared to the changes in gas-to-particle partitioning brought by the use of EQSAM4Clim. [ABSTRACT FROM AUTHOR]

We use an inorganic aerosol thermodynamic equilibrium model in a three-dimensional chemical transport model to understand the roles of ammonia chemistry and natural aerosols on the global distribution of aerosols. The thermodynamic equilibrium model partitions gas-phase precursors among modeled aerosol species self-consistently with ambient relative humidity and natural and anthropogenic aerosol emissions during the 1990s.Model simulations show that accounting for aerosol inorganic thermodynamic equilibrium, ammonia chemistry and dust and sea-salt aerosols improve agreement with observed SO4, NO3, and NH4 aerosols especially at North American sites. This study shows that the presence of sea salt, dust aerosol and ammonia chemistry significantly increases sulfate over polluted continental regions. In all regions and seasons, representation of ammonia chemistry is required to obtain reasonable agreement between modeled and observed sulfate and nitrate concentrations. Observed and modeled correlations of sulfate and nitrate with ammonium confirm that the sulfate and nitrate are strongly coupled with ammonium. SO4concentrations over East China peak in winter, while North American SO4 peaks in summer. Seasonal variations of NO3 and SO4 are the same in East China. In North America, the seasonal variation is much stronger for NO3 than SO4 and peaks in winter.Natural sea salt and dust aerosol significantly alter the regional distributions of other aerosols in three main ways. First, they increase sulfate formation by 10–70% in polluted areas. Second, they increase modeled nitrate over oceans and reduce nitrate over Northern hemisphere continents. Third, they reduce ammonium formation over oceans and increase ammonium over Northern Hemisphere continents. Comparisons of SO4, NO3 and NH4 deposition between pre-industrial, present, and year 2100 scenarios show that the present NO3and NH4 deposition are twice pre-industrial deposition and present SO4 deposition is almost five times pre-industrial deposition.

The Equilibrium Simplified Aerosol Model for Climate version 12 (EQSAM4Clim-v12) has recently been revised to provide an accurate and efficient method for calculating the acidity of atmospheric particles. EQSAM4Clim is based on an analytical concept that is not only sufficiently fast for numerical weather prediction (NWP) applications, but also free of numerical noise, which makes it attractive also for air quality forecasting. EQSAM4Clim allows the calculation of aerosol composition based on the gas-liquid-solid and the reduced gas-liquid partitioning with the associated water uptake for both cases, and can therefore provide important information about the acidity of the aerosols. Here we provide a comprehensive description of the recent changes made to the aerosol acidity parameterization (referred to a version 12) which builds on the original EQSAM4Clim. We evaluate the pH improvements using a detailed box-model and compare against previous model calculations and both ground-based and aircraft observations from US and China covering different seasons and scenarios. We show that, in most cases, the simulated pH is within reasonable agreement with the results of the E-AIM reference model and of satisfactory accuracy. [ABSTRACT FROM AUTHOR]

To improve the aeolian dust budget calculations with the global ECHAM/MESSy atmospheric chemistry-climate model (EMAC) we have implemented new input data and updates of the emission scheme. The data set comprises landcover classification, vegetation, clay fraction and topography. It is based on up-to-date observations, which is crucial to account for the rapid changes of deserts and semi-arid regions in recent decades. The new Moderate-resolution Imaging Spectroradiometer (MODIS) based landcover and vegetation data is time dependent, and the effect of long-term trends and variability of the relevant parameters is therefore considered by the emission scheme. All input data has a spatial resolution of at least 0.1° compared to 1° in the previous version, equipping the model for high resolution simulations. We validate the updates by comparing results for the aerosol optical depth (AOD) at 550 nm wavelength from a one year simulation at T106 (about 1.1°) resolution with Aerosol Robotic Network (AERONET) and MODIS observations, and results for 10 μm dust AOD (DAOD) with Infrared Atmospheric Sounding Interferometer (IASI) retrievals. The update significantly improves agreement with the observations and is therefore recommended to be used in future simulations. [ABSTRACT FROM AUTHOR]

We use the combined Dark Target/Deep Blue aerosol optical depth (AOD) satellite product of the moderate-resolution imaging spectroradiometer (MODIS) collection 6 to study trends over the Middle East between 2000 and 2015. Our analysis corroborates a previously identified positive AOD trend over large parts of the Middle East during the period 2001 to 2012. We relate the annual AOD to precipitation, soil moisture and surface winds to identify regions where these attributes are directly related to the AOD over Saudi Arabia, Iraq and Iran. Regarding precipitation and soil moisture, a relatively small area in and surrounding Iraq turns out to be of prime importance for the AOD over these countries. Regarding surface wind speed, the African Red Sea coastal area is relevant for the Saudi Arabian AOD. Using multiple linear regression we show that AOD trends and interannual variability can be attributed to soil moisture, precipitation and surface winds, being the main factors controlling the dust cycle. Our results confirm the dust driven AOD trends and variability, supported by a decreasing MODIS-derived Ångström exponent and a decreasing AERONET-derived fine mode fraction that accompany the AOD increase over Saudi Arabia. The positive AOD trend relates to a negative soil moisture trend. As a lower soil moisture translates into enhanced dust emissions, it is not needed to assume growing anthropogenic aerosol and aerosol precursor emissions to explain the observations. Instead, our results suggest that increasing temperature and decreasing relative humidity in the last decade have promoted soil drying, leading to increased dust emissions and AOD; consequently an AOD increase is expected due to climate change. [ABSTRACT FROM AUTHOR]