Atmos. Chem. Phys. Discuss., 11, 22801-22856, 2011
www.atmos-chem-phys-discuss.net/11/22801/2011/
doi:10.5194/acpd-11-22801-2011
© Author(s) 2011. This work is distributed
under the Creative Commons Attribution 3.0 License.
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Immersion mode heterogeneous ice nucleation by an illite rich powder representative of atmospheric mineral dust
S. L. Broadley, B. J. Murray, R. J. Herbert, J. D. Atkinson, S. Dobbie, E. Condliffe, and L. Neve
School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK

Abstract. Atmospheric dust rich in illite is transported globally from arid regions and may impact cloud properties through the nucleation of ice. We present measurements of ice nucleation in water droplets containing known quantities of an illite rich powder under atmospherically relevant conditions. The illite rich powder used here, NX illite, has a similar mineralogical composition to atmospheric mineral dust sampled in remote locations, i.e. dust which has been subject to long range transport, cloud processing and sedimentation. Arizona Test Dust has a significantly different mineralogical composition and we suggest that NX illite is a better surrogate of natural atmospheric dust. Heterogeneous nucleation by NX illite was observed, using optical microscopy, to occur dominantly between 246 K and the homogeneous freezing limit and higher freezing temperatures were observed with larger surface areas of NX illite present within the droplets. It is shown that there is strong particle to particle variability in terms of ice nucleating ability with a few particles dominating ice nucleation at high surface areas. In fact, this work suggests that the bulk of atmospheric mineral dust particles are less efficient at nucleating ice than assumed in parameterisation currently used in models. For droplets containing ≤2 × 10−6 cm2 of NX illite, freezing temperatures did not noticeably change when the cooling rate was varied by an order of magnitude. The data obtained during cooling experiments (with surface areas ≤2 × 10−6 cm2) is shown to be inconsistent with the single component stochastic model, but is well described by the singular model (ns(236.2 K ≤ T ≤ 247.5 K) = exp(6.53043 × 104 − 8.2153088 × 102 T + 3.446885376 T 2 − 4.822268 × 10−3 T3). However, droplets continued to freeze when the temperature was held constant, which is inconsistent with the time independent singular model. We show that this apparent discrepancy can be resolved using a multiple component stochastic model in which it is assumed there are many types of nucleation sites, each with a unique temperature dependent nucleation coefficient. Cooling rate independence can be achieved with this time dependent model if the nucleation rate coefficients increase very rapidly with decreasing temperature, thus reconciling our measurement of nucleation at constant temperature with the cooling rate independence.

Citation: Broadley, S. L., Murray, B. J., Herbert, R. J., Atkinson, J. D., Dobbie, S., Condliffe, E., and Neve, L.: Immersion mode heterogeneous ice nucleation by an illite rich powder representative of atmospheric mineral dust, Atmos. Chem. Phys. Discuss., 11, 22801-22856, doi:10.5194/acpd-11-22801-2011, 2011.
 
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