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Primary versus secondary contributions to particle number concentrations in the European boundary layer

2011, Reddington, C.L., Carslaw, K.S., Spracklen, D.V., Frontoso, M.G., Collins, L., Merikanto, J., Minikin, A., Hamburger, T., Coe, H., Kulmala, M., Aalto, P., Flentje, H., Plass-Dülmer, C., Birmili, W., Wiedensohler, A., Wehner, B., Tuch, T., Sonntag, A., O'Dowd, C.D., Jennings, S.G., Dupuy, R., Baltensperger, U., Weingartner, E., Hansson, H.-C., Tunved, P., Laj, P., Sellegri, K., Boulon, J., Putaud, J.-P., Gruening, C., Swietlicki, E., Roldin, P., Henzing, J.S., Moerman, M., Mihalopoulos, N., Kouvarakis, G., Ždímal, V., Zíková, N., Marinoni, A., Bonasoni, P., Duchi, R.

It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.

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Atmospheric data over a solar cycle: No connection between galactic cosmic rays and new particle formation

2010, Kulmala, M., Riipinen, I., Nieminen, T., Hulkkonen, M., Sogacheva, L., Manninen, H.E., Paasonen, P., Petäjä, T., Dal Maso, M., Aalto, P.P., Viljanen, A., Usoskin, I., Vainio, R., Mirme, S., Mirme, A., Minikin, A., Petzold, A., Hõrrak, U., Plaß-Dülmer, C., Birmili, W., Kerminen, V.-M.

Aerosol particles affect the Earth's radiative balance by directly scattering and absorbing solar radiation and, indirectly, through their activation into cloud droplets. Both effects are known with considerable uncertainty only, and translate into even bigger uncertainties in future climate predictions. More than a decade ago, variations in galactic cosmic rays were suggested to closely correlate with variations in atmospheric cloud cover and therefore constitute a driving force behind aerosol-cloud-climate interactions. Later, the enhancement of atmospheric aerosol particle formation by ions generated from cosmic rays was proposed as a physical mechanism explaining this correlation. Here, we report unique observations on atmospheric aerosol formation based on measurements at the SMEAR II station, Finland, over a solar cycle (years 1996–2008) that shed new light on these presumed relationships. Our analysis shows that none of the quantities related to aerosol formation correlates with the cosmic ray-induced ionisation intensity (CRII). We also examined the contribution of ions to new particle formation on the basis of novel ground-based and airborne observations. A consistent result is that ion-induced formation contributes typically significantly less than 10% to the number of new particles, which would explain the missing correlation between CRII and aerosol formation. Our main conclusion is that galactic cosmic rays appear to play a minor role for atmospheric aerosol formation events, and so for the connected aerosol-climate effects as well.

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Spectral surface albedo over Morocco and its impact on radiative forcing of Saharan dust

2009, Bierwirth, E., Wendisch, M., Ehrlich, A., Heese, B., Tesche, M., Althausen, D., Schladitz, A., Müller, D., Otto, S., Trautmann, T., Dinter, T., Von Hoyningen-Huene, W., Kahn, R.

In May-June 2006, airborne and ground-based solar (0.3-2.2 μm) and thermal infrared (4-42 μm) radiation measurements have been performed in Morocco within the Saharan Mineral Dust Experiment (SAMUM). Upwelling and downwelling solar irradiances have been measured using the Spectral Modular Airborne Radiation Measurement System (SMART)-Albedometer. With these data, the areal spectral surface albedo for typical surface types in southeastern Morocco was derived from airborne measurements for the first time. The results are compared to the surface albedo retrieved from collocated satellite measurements, and partly considerable deviations are observed. Using measured surface and atmospheric properties, the spectral and broad-band dust radiative forcing at top-of-atmosphere (TOA) and at the surface has been estimated. The impact of the surface albedo on the solar radiative forcing of Saharan dust is quantified. In the SAMUM case of 19 May 2006, TOA solar radiative forcing varies by 12 W m-2 per 0.1 surface-albedo change. For the thermal infrared component, values of up to +22 W m-2 were derived. The net (solar plus thermal infrared) TOA radiative forcing varies between -19 and +24 W m-2 for a broad-band solar surface albedo of 0.0 and 0.32, respectively. Over the bright surface of southeastern Morocco, the Saharan dust always has a net warming effect. © 2008 The Author Journal compilation © 2008 Blackwell Munksgaard.