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Limited impact of sulfate-driven chemistry on black carbon aerosol aging in power plant plumes

1 Earth System Research Laboratory, Chemical Sciences Division, NOAA, Boulder, Colorado, USA
2 Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Colorado, USA
3 Department of Physics, University of Oxford, Oxford, Oxfordshire, United Kingdom
4 Now at Picarro Inc, Santa Clara, CA, USA
5 Now at Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, Maryland, and Universities Space Research Association, GESTAR, Columbia, Maryland
6 Now at Finnish Meteorological Institute, Helsinki, Finland
7 Now at Department of Atmospheric Science, Colorado State University, Ft. Collins, Colorado, USA

The aging of refractory black carbon (rBC) aerosol by sulfate-driven chemistry has been constrained in coal-fired power-plant plumes using the NOAA WP-3D research aircraft during the Southern Nexus (SENEX) study, which took place in the Southeastern US in June and July of 2013. A Single Particle Soot Photometer (SP2) determined the microphysical properties of rBC-containing particles including single-particle rBC mass and the presence and amount of internally-mixed non-rBC material, hereafter referred to as “coatings”. Most power-plant influenced air was associated with very slightly increased amounts of non-refractory material, likely sulfate internally mixed with the rBC, however this increase was statistically insignificant even after semi-Lagrangian exposure for up to 5 h. On average, the increase in coating thickness was 2 ± 4 nm for particles containing 3–5 fg rBC. Similarly, the number fraction of rBC-containing particles that could be identified as internally mixed was increased by plume chemistry by only 1.3 ± 1.3%. These direct measurements of microphysical aging of rBC-containing aerosol by power plant emissions constrain the enhancement of sulfate chemistry on both rBC’s column-integrated absorption optical depth, and rBC-containing aerosol’s ability to act as cloud condensation nuclei. Appling Mie and k-Köhler theories to the SP2 observations, permits the resulting effect on rBC ambient light-absorption to be capped at the 2–6% level.
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