Laboratory studies of ice formation pathways from ammonium sulfate particles

Abstract. Cirrus clouds are composed of ice particles and their formation pathways have been studied extensively in the laboratory. The ability of ammonium sulfate particles to act as nuclei for cirrus clouds has been of particular importance because of their ubiquitous presence in the upper troposphere. The results of past laboratory experiments of homogeneous ice nucleation from ammonium sulfate particles show a wide range of freezing conditions. In the present study, a flow tube apparatus equipped with Fourier transform infrared spectroscopy was used to resolve these discrepancies. It was found that when ammonium sulfate particles were preconditioned at 100% relative humidity (RH) prior to experimentation, the particles froze at conditions predicted by the homogeneous ice nucleation model developed by Koop et al. (2000). If the particles were not preconditioned at 100% RH, they froze at warmer temperatures and lower ice saturation ratios than predicted by Koop et al. (2000). In order to determine if a population of effloresced particles affected freezing conditions for particles that were not preconditioned at 100% RH, a series of depositional ice nucleation experiments were carried out on dry ammonium sulfate particles. For freezing temperatures between 215 and 231 K, ice nucleated on the particles at ice saturation ratios (Sice) between 1 and 1.05. These conditions are much lower than predicted by Koop et al. (2000) and explain the differences in freezing conditions among preconditioning methods. In similar experiments, Abbatt et al. (2006) hypothesized that a small fraction of effloresced ammonium sulfate particles induced ice nucleation at Sice values lower than expected. The current study confirms the Abbatt et al. (2006) hypothesis and, to our knowledge, is the first study to directly observe ice nucleating onto freely flowing dry ammonium sulfate particles at Sice values approaching unity.