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Volume 16, issue 10
Atmos. Chem. Phys., 16, 6511–6535, 2016
https://doi.org/10.5194/acp-16-6511-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Special issue: Carbonaceous Aerosols and Radiative Effects Study (CARES)

Atmos. Chem. Phys., 16, 6511–6535, 2016
https://doi.org/10.5194/acp-16-6511-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 27 May 2016

Research article | 27 May 2016

Understanding the optical properties of ambient sub- and supermicron particulate matter: results from the CARES 2010 field study in northern California

Christopher D. Cappa1, Katheryn R. Kolesar1,a, Xiaolu Zhang1, Dean B. Atkinson2, Mikhail S. Pekour3, Rahul A. Zaveri3, Alla Zelenyuk4, and Qi Zhang5 Christopher D. Cappa et al.
  • 1Department of Civil and Environmental Engineering, University of California, Davis, CA 95616, USA
  • 2Department of Chemistry, Portland State University, Portland, OR 92707, USA
  • 3Atmospheric Sciences & Global Change Division, Pacific Northwest National Laboratory, Richland, WA 99352, USA
  • 4Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99352, USA
  • 5Department of Environmental Toxicology, University of California, Davis, CA 95616, USA
  • anow at: Department of Chemistry, University of Michigan, Ann Arbor, MI 48109, USA

Abstract. Measurements of the optical properties (absorption, scattering and extinction) of PM1, PM2.5 and PM10 made at two sites around Sacramento, CA, during the June 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) are reported. These observations are used to establish relationships between various intensive optical properties and to derive information about the dependence of the optical properties on photochemical aging and sources. Supermicron particles contributed substantially to the total light scattering at both sites, about 50 % on average. A strong, linear relationship is observed between the scattering Ångström exponent for PM10 and the fraction of the scattering that is contributed by submicron particles (fsca, PM1) at both sites and with similar slopes and intercepts (for a given pair of wavelengths), suggesting that the derived relationship may be generally applicable for understanding variations in particle size distributions from remote sensing measurements. At the more urban T0 site, the fsca, PM1 increased with photochemical age, whereas at the downwind, more rural T1 site the fsca, PM1 decreased slightly with photochemical age. This difference in behavior reflects differences in transport, local production and local emission of supermicron particles between the sites. Light absorption is dominated by submicron particles, but there is some absorption by supermicron particles ( ∼  15 % of the total). The supermicron absorption derives from a combination of black carbon that has penetrated into the supermicron mode and from dust, and there is a clear increase in the mass absorption coefficient of just the supermicron particles with increasing average particle size. The mass scattering coefficient (MSC) for the supermicron particles was directly observed to vary inversely with the average particle size, demonstrating that MSC cannot always be treated as a constant in estimating mass concentrations from scattering measurements, or vice versa. The total particle backscatter fraction exhibited some dependence upon the relative abundance of sub- versus supermicron particles; however this was modulated by variations in the median size of particles within a given size range; variations in the submicron size distribution had a particularly large influence on the observed backscatter efficiency and an approximate method to account for this variability is introduced. The relationship between the absorption and scattering Ångström exponents is examined and used to update a previously suggested particle classification scheme. Differences in composition led to differences in the sensitivity of PM2.5 to heating in a thermodenuder to the average particle size, with more extensive evaporation (observed as a larger decrease in the PM2.5 extinction coefficient) corresponding to smaller particles; i.e., submicron particles were generally more susceptible to heating than the supermicron particles. The influence of heating on the particle hygroscopicity varied with the effective particle size, with larger changes observed when the PM2.5 distribution was dominated by smaller particles.

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Measurements of size-dependent aerosol optical properties at visible wavelengths made during the 2010 CARES study are reported on, with a special focus on the characterization of supermicron particles. The relationships with and dependence upon particle composition, particle size, photochemical aging, water uptake and heating are discussed, along with broader implications of these in situ measurements for the interpretation of remote sensing products.
Measurements of size-dependent aerosol optical properties at visible wavelengths made during the...
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