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Discussion papers
https://doi.org/10.5194/acp-2018-915
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-915
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 17 Sep 2018

Research article | 17 Sep 2018

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Laboratory study of the heterogeneous ice nucleation on black carbon containing aerosol

Leonid Nichman1,4, Martin Wolf2, Paul Davidovits1, Timothy B. Onasch1,4, Yue Zhang1,4,5, Doug R. Worsnop4, Janarjan Bhandari6, Claudio Mazzoleni6, and Daniel J. Cziczo2,3 Leonid Nichman et al.
  • 1Department of Chemistry, Boston College, Chestnut Hill, MA, 02467, USA
  • 2Department of Earth, Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA, USA
  • 3Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA
  • 4Aerodyne Research, Inc, Billerica, MA, 01821, USA
  • 5Department of Environmental Science and Engineering, Gillings School of Global Public Health, University of North Carolina at Chapel Hill, Chapel Hill, NC, 27599, USA
  • 6Department of Physics and Atmospheric Sciences Program, Michigan Technological University, Houghton, MI, 49931, USA

Abstract. Black carbon (BC) particles are generated in the incomplete combustion of fossil fuels, biomass, and biofuels. These airborne particles affect air quality, human health, and climate. At present, the climate effects of BC particles are not well understood. Their role in cloud formation is obscured by their chemical and physical variability, and by the internal mixing states of these particles with other compounds. The current study focuses on laboratory measurements of the effectiveness of BC-containing aerosol in the formation of ice crystals in cirrus clouds. Ice nucleation in field studies is often difficult to interpret. Nonetheless, most field studies seem to suggest that BC particles are not efficient ice nuclei (IN). On the other hand, laboratory measurements show that in some cases, BC particles can be highly active IN. By working with well-characterized BC-containing particles, our aim is to systematically establish the factors that govern the IN activity of BC.

We examine ice nucleation on BC-containing particles under cirrus cloud conditions, commonly understood to be deposition mode ice nucleation. We study a series of well-characterized commercial carbon black particles with varying morphologies and surface chemistries, as well as ethylene flame-generated combustion soot. The carbon black particles used in this study are proxies for atmospherically relevant BC aerosols. These samples were characterized by electron microscopy, mass spectrometry, and optical scattering measurements. Ice nucleation activity was systematically examined in the temperature range from 217–235K, using a SPectrometer for Ice Nuclei (SPIN) instrument, which is a continuous flow diffusion chamber coupled with instrumentation to measure light scattering and polarization. To study the effect of coatings on IN, the BC-containing particles were coated with organic acids found in the atmosphere, namely, stearic acid, cis-pinonic acid, and oxalic acid.

The results show significant variations in ice nucleation activity as a function of size, morphology and surface chemistry of the BC-containing particles. The measured IN activity dependence on temperature and the physicochemical properties of the BC-containing particles are consistent with an ice nucleation mechanism of pore condensation followed by freezing. Coatings and surface oxidation modify the initial ice nucleation ability of BC-containing aerosol. Depending on the BC material and the coating, both inhibition and enhancement in IN activity were observed. Our measurements at low temperatures complement published data, and highlight the capability of some BC particles to nucleate ice under low supersaturation conditions. These results are expected to help refine theories relating to soot IN activation in the atmosphere.

Leonid Nichman et al.
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Short summary
Previous studies showed widespread ice nucleation activity of soot. In this systematic study we investigated the factors that affect the heterogeneous ice nucleation activity of soot surrogates in the cirrus cloud regime. Our observations are consistent with an ice nucleation mechanism of pore condensation followed by freezing. The results show significant variations in ice nucleation activity as a function of size, morphology and surface chemistry of the black carbon containing particles.
Previous studies showed widespread ice nucleation activity of soot. In this systematic study we...
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