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We evaluate, using a box model, the sensitivity of direct climate forcing by atmospheric aerosols for a “global mean” aerosol that consists of fine and coarse modes to aerosol composition, aerosol size distribution, relative humidity (RH), aerosol mixing state (internal versus external mixture), deliquescence/crystallization hysteresis, and solar zenith angle. We also examine the dependence of aerosol upscatter fraction on aerosol size, solar zenith angle, and wavelength and the dependence of single scatter albedo on wavelength and aerosol composition. The single most important parameter in determining direct aerosol forcing is relative humidity, and the most important process is the increase of the aerosol mass as a result of water uptake. An increase of the relative humidity from 40 to 80% is estimated for the global mean aerosol considered to result in an increase of the radiative forcing by a factor of 2.1. Forcing is relatively insensitive to the fine mode diameter increase due to hygroscopic growth, as long as this mode remains inside the efficient scattering size region. The hysteresis/deliquescence region introduces additional uncertainty but, in general, errors less than 20% result by the use of the average of the two curves to predict forcing. For fine aerosol mode mean diameters in the 0.2–0.5 μm range direct aerosol forcing is relatively insensitive (errors less than 20%) to variations of the mean diameter. Estimation of the coarse mode diameter within a factor of 2 is generally sufficient for the estimation of the total aerosol radiative forcing within 20%. Moreover, the coarse mode, which represents the nonanthropogenic fraction of the aerosol, is estimated to contribute less than 10% of the total radiative forcing for all RHs of interest. Aerosol chemical composition is important to direct radiative forcing as it determines (1) water uptake with RH, and (2) optical properties. The effect of absorption by aerosol components on forcing is found to be significant even for single scatter albedo values of ω=0.93–0.97. The absorbing aerosol component reduces the aerosol forcing from that in its absence by roughly 30% at 60% RH and 20% at 90% RH. The mixing state of the aerosol (internal versus external) for the particular aerosol considered here is found to be of secondary importance. While sulfate mass scattering efficiency (m2 (g SO42−)−1) and the normalized sulfate forcing (W (g SO42−)−1) increase strongly with RH, total mass scattering efficiency (m2 g−1) and normalized forcing (W g−1) are relatively insensitive to RH, wherein the mass of all species, including water, are accounted for. Following S. Nemesure et al. (Direct shortwave forcing of climate by anthropogenic sulfate aerosol: sensitivity to particle size, composition, and relative humidity, submitted to Journal of Geophysical Research, 1995), we find that aerosol feeing achieves a maximum at a particular solar zenith angle, reflecting a balance between increasing upscatter fraction with increasing solar zenith angle and decreasing solar flux...

Abstract. In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

Abstract. 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 1 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 1 species in cenCorrespondence to: S. N. Pandis (spyros@andrew.cmu.edu) tral 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 1 OA. The model tends to predict relatively flat diurnal profiles for PM 1 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.