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Uncertainties of simulated aerosol optical properties induced by assumptions on aerosol physical and chemical properties: An AQMEII-2 perspective
2014, Curci, G., Hogrefe, C., Bianconi, R., Im, U., Balzarini, A., Baró, R., Brunner, D., Forkel, R., Giordano, L., Hirtl, M., Honzak, L., Jiménez-Guerrero, P., Knote, C., Langer, M., Makar, P.A., Pirovano, G., Pérez, J.L., San José, R., Syrakov, D., Tuccella, P., Werhahn, J., Wolke, R., Žabkar, R., Zhang, J., Galmarini, S.
The calculation of aerosol optical properties from aerosol mass is a process subject to uncertainty related to necessary assumptions on the treatment of the chemical species mixing state, density, refractive index, and hygroscopic growth. In the framework of the AQMEII-2 model intercomparison, we used the bulk mass profiles of aerosol chemical species sampled over the locations of AERONET stations across Europe and North America to calculate the aerosol optical properties under a range of common assumptions for all models. Several simulations with parameters perturbed within a range of observed values are carried out for July 2010 and compared in order to infer the assumptions that have the largest impact on the calculated aerosol optical properties. We calculate that the most important factor of uncertainty is the assumption about the mixing state, for which we estimate an uncertainty of 30–35% on the simulated aerosol optical depth (AOD) and single scattering albedo (SSA). The choice of the core composition in the core–shell representation is of minor importance for calculation of AOD, while it is critical for the SSA. The uncertainty introduced by the choice of mixing state choice on the calculation of the asymmetry parameter is the order of 10%. Other factors of uncertainty tested here have a maximum average impact of 10% each on calculated AOD, and an impact of a few percent on SSA and g. It is thus recommended to focus further research on a more accurate representation of the aerosol mixing state in models, in order to have a less uncertain simulation of the related optical properties.
A European aerosol phenomenology - 7: High-time resolution chemical characteristics of submicron particulate matter across Europe
2021, Bressi, M., Cavalli, F., Putaud, J.P., Fröhlich, R., Petit, J.-E., Aas, W., Äijälä, M., Alastuey, A., Allan, J.D., Aurela, M., Berico, M., Bougiatioti, A., Bukowiecki, N., Canonaco, F., Crenn, V., Dusanter, S., Ehn, M., Elsasser, M., Flentje, H., Graf, P., Green, D.C., Heikkinen, L., Hermann, H., Holzinger, R., Hueglin, C., Keernik, H., Kiendler-Scharr, A., Kubelová, L., Lunder, C., Maasikmets, M., Makeš, O., Malaguti, A., Mihalopoulos, N., Nicolas, J.B., O'Dowd, C., Ovadnevaite, J., Petralia, E., Poulain, L., Priestman, M., Riffault, V., Ripoll, A., Schlag, P., Schwarz, J., Sciare, J., Slowik, J., Sosedova, Y., Stavroulas, I., Teinemaa, E., Via, M., Vodička, P., Williams, P.I., Wiedensohler, A., Young, D.E., Zhang, S., Favez, O., Minguillón, M.C., Prevot, A.S.H.
Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62°N and 10° W – 26°E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36–64%) of NR-PM1 followed by sulfate (12–44%) and nitrate (6–35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in mid-latitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (μg/m³) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 μg/m³ at half of the sites. © 2021 The Authors