Atmospheric Chemistry and Physics (Sep 2011)

Studies of propane flame soot acting as heterogeneous ice nuclei in conjunction with single particle soot photometer measurements

  • I. Crawford,
  • O. Möhler,
  • M. Schnaiter,
  • H. Saathoff,
  • D. Liu,
  • G. McMeeking,
  • C. Linke,
  • M. Flynn,
  • K. N. Bower,
  • P. J. Connolly,
  • M. W. Gallagher,
  • H. Coe

DOI
https://doi.org/10.5194/acp-11-9549-2011
Journal volume & issue
Vol. 11, no. 18
pp. 9549 – 9561

Abstract

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The ice nucleation efficiency of propane flame soot particles with and without a sulphuric acid coating was investigated using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere). The test soot for cloud formation simulations was produced using a propane flame Combustion Aerosol Standard generator (CAST, Jing-CAST Technologies). The organic carbon content (OC) of the test soot was altered in a reproducible fashion by changing the fuel/air mixture of the generator. The soot content of ice nuclei was subsequently investigated using a combination of a pumped counterflow virtual impactor (PCVI) to separate and evaporate the ice crystals, and a DMT single particle soot photometer (SP2) to examine the mixing state of the BC containing ice residuals. <br><br> Ice nucleation was found to be most efficient for uncoated soot of low organic carbon content (~5 % organic carbon content) where deposition freezing occurred at an ice saturation ratio <i>S</i><sub>ice</sub> ~ 1.22 at a temperature <i>T</i> = 226.6 K with 25 % of the test soot becoming active as ice nuclei. Propane flame soot of higher organic carbon content (~30 % and ~70 % organic carbon content) showed significantly lower ice nucleation efficiency (an activated fraction of the order of a few percent in the experiments) than the low organic carbon content soot, with water saturation being required for freezing to occur. Ice nucleation occurred over the range <i>S</i><sub>ice</sub> = 1.22–1.70, and <i>T</i> = 223.2–226.6 K. Analysis of the SP2 data showed that the 5 % organic carbon content soot had an undetectable OC coating whereas the 30 % organic carbon content soot had a thicker or less volatile OC coating. <br><br> The application of a sulphuric acid coating to the flame soot shifted the threshold of the onset of freezing towards that of the homogeneous freezing of sulphuric acid; for the minimum OC flame soot this inhibited nucleation since the onset of freezing occurred at colder temperatures and required a greater ice saturation ratio; for the medium and maximum OC flame soot, the addition of a sulphuric acid significantly reduced the freezing threshold.