Abstract

Abstract. Kaolinite particles from two different sources (Fluka and Clay Minerals Society (CMS)) were examined with respect to their ability to act as ice nuclei (IN). This was done in the water-subsaturated regime where often deposition ice nucleation is assumed to occur, and for water-supersaturated conditions, i.e., in the immersion freezing mode. Measurements were done using a flow tube (the Leipzig Aerosol Cloud Interaction Simulator, LACIS) and a continuous-flow diffusion chamber (CFDC). Pure and coated particles were used, with coating thicknesses of a few nanometers or less, where the coating consisted of levoglucosan, succinic acid or sulfuric acid. In general, it was found that the coatings strongly reduced deposition ice nucleation. Remaining ice formation in the water-subsaturated regime could be attributed to immersion freezing, with particles immersed in concentrated solutions formed by the coatings. In the immersion freezing mode, ice nucleation rate coefficients jhet from both instruments agreed well with each other, particularly when the residence times in the instruments were accounted for. Fluka kaolinite particles coated with either levoglucosan or succinic acid showed the same IN activity as pure Fluka kaolinite particles; i.e., it can be assumed that these two types of coating did not alter the ice-active surface chemically, and that the coatings were diluted enough in the droplets that were formed prior to the ice nucleation, so that freezing point depression was negligible. However, Fluka kaolinite particles, which were either coated with pure sulfuric acid or were first coated with the acid and then exposed to additional water vapor, both showed a reduced ability to nucleate ice compared to the pure particles. For the CMS kaolinite particles, the ability to nucleate ice in the immersion freezing mode was similar for all examined particles, i.e., for the pure ones and the ones with the different types of coating. Moreover, jhet derived for the CMS kaolinite particles was comparable to jhet derived for Fluka kaolinite particles coated with sulfuric acid. This is suggestive for the Fluka kaolinite possessing a type of ice-nucleating surface feature which is not present on the CMS kaolinite, and which can be destroyed by reaction with sulfuric acid. This might be potassium feldspar.

Highlights

  • Ice in clouds is a research topic which received interest already before the 1950s

  • Following Koop and Zobrist (2009) and the literature cited therein, λhom can be expected to be on the order of 2 to 2.5 for the soluble substances we examined in our study

  • Freezing measurements were done using two different instruments, LACIS (Hartmann et al, 2011) and a continuous-flow diffusion chamber (CFDC) (DeMott et al, 2010), where both instruments measured in the water-supersaturated regime, while deposition ice nucleation or other mechanisms possible in the water-subsaturated regime were only examined by the CFDC

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Summary

Introduction

Ice in clouds is a research topic which received interest already before the 1950s (see e.g. Vonnegut, 1947). The present study extends from Tobo et al (2012) It includes a comparison of the measured immersion freezing by LACIS and the CFDC, additional data on CMS (Clay Minerals Society) kaolinite and data on coatings with succinic acid. It discusses a model for describing the heterogeneous ice formation of particles with sufficiently thick coatings at relative humidities below 100 %, interpreting this type of freezing as immersion freezing of IN immersed in concentrated solutions. Fice, from the CFDC measurements, measured total particle number concentrations were used together with the IN number concentrations; i.e., the same parameter was derived that was obtained from the LACIS measurements

Coating thicknesses
Immersion freezing
Ice nucleation under water-subsaturated conditions
Summary and conclusions
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