Abstract

Abstract. We investigated the ice nucleating properties of mineral dust particles to understand the sensitivity of simulated cloud properties to two different representations of contact angle in the Classical Nucleation Theory (CNT). These contact angle representations are based on two sets of laboratory deposition ice nucleation measurements: Arizona Test Dust (ATD) particles of 100, 300 and 500 nm sizes were tested at three different temperatures (−25, −30 and −35 °C), and 400 nm ATD and kaolinite dust species were tested at two different temperatures (−30 and −35 °C). These measurements were used to derive the onset relative humidity with respect to ice (RHice) required to activate 1% of dust particles as ice nuclei, from which the onset single contact angles were then calculated based on CNT. For the probability density function (PDF) representation, parameters of the log-normal contact angle distribution were determined by fitting CNT-predicted activated fraction to the measurements at different RHice. Results show that onset single contact angles vary from ~18 to 24 degrees, while the PDF parameters are sensitive to the measurement conditions (i.e. temperature and dust size). Cloud modeling simulations were performed to understand the sensitivity of cloud properties (i.e. ice number concentration, ice water content, and cloud initiation times) to the representation of contact angle and PDF distribution parameters. The model simulations show that cloud properties are sensitive to onset single contact angles and PDF distribution parameters. The comparison of our experimental results with other studies shows that under similar measurement conditions the onset single contact angles are consistent within ±2.0 degrees, while our derived PDF parameters have larger discrepancies.

Highlights

  • Ice containing clouds constitute one of the largest sources of uncertainty in predicting the Earth’s climate according to the Intergovernmental Panel on Climate Change (IPCC) 2007 report (Forster et al, 2007)

  • We experimentally investigate the ice nucleating properties of mineral dust particles and examine the impact of the nucleation properties within the original and modified Classical Nucleation Theory (CNT) framework on cloud properties simulated with an offline module and a cloud resolving model (CRM)

  • Ice nucleates on the aerosol particles and the newly formed ice crystal grows to a size greater than the original aerosol size, and ice crystals greater than 1 micrometer exiting the chamber are counted with an optical particle counter (OPC; CLiMET, model CI-3100)

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Summary

Introduction

Ice containing clouds constitute one of the largest sources of uncertainty in predicting the Earth’s climate according to the Intergovernmental Panel on Climate Change (IPCC) 2007 report (Forster et al, 2007). There are at least two reasons why heterogeneous ice nucleation is much more complex than homogeneous freezing. It requires special atmospheric aerosols, called ice nuclei (IN) (Pruppacher and Klett, 1997), which lower the free energy barrier for ice nucleation. Aerosol surface characteristics, such as morphology, solubility, active sites and epitaxial properties, have been postulated to play important roles in determining the IN efficiency of aerosol particles, but formulating a relationship among these characteristics has been difficult. There are multiple heterogeneous ice nucleation mechanisms observed or hypothesized (Vali, 1985), such as deposition nucleation

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