1Centre for Atmospheric Science, University of Manchester, Manchester, UK
2Department of Meteorology, University of Reading, Reading, UK
3The Met Office, Exeter, UK
4CEMPS, University of Exeter, Exeter, UK
*now at: Dept. of Atmospheric Science, Colorado State University, Fort Collins, CO, USA
Received: 27 Apr 2011 – Discussion started: 17 May 2011
Abstract. Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in urban plumes compared to regional aerosol (0.85 versus 0.9–0.95). We attribute these differences to the presence of relatively rapidly formed secondary aerosol, primarily OOA and ammonium nitrate, which must be taken into account in radiative forcing calculations.
Revised: 08 Aug 2011 – Accepted: 29 Aug 2011 – Published: 05 Sep 2011
McMeeking, G. R., Morgan, W. T., Flynn, M., Highwood, E. J., Turnbull, K., Haywood, J., and Coe, H.: Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom, Atmos. Chem. Phys., 11, 9037-9052, doi:10.5194/acp-11-9037-2011, 2011.