Numerical Simulations of Homogeneous Freezing Processes in the Aerosol Chamber AIDA

ATMOSPHERIC CHEMISTRY AND PHYSICS (Impact Factor: 5.51). 01/2002; 3(2003):195-210. DOI: 10.5194/acp-3-195-2003
Source: DLR

ABSTRACT The homogeneous freezing of supercooled H2SO4/H2O aerosols in an aerosol chamber is investigated with a microphysical box model using the activity parameterization of the nucleation rate by Koop et al (2000). The simulations are constrained by measurements of pressure, temperature, total water mixing ratio, and the initial aerosol size distribution, described in a companion paper Möhler et al. (2002). Model results are compared to measurements conducted in the temperature range between 194 and 235 K, with cooling rates in the range between 0.5 and 2.6 K min-1, and at air pressures between 170 and 1000 hPa. The simulations focus on the time history of relative humidity with respect to ice, aerosol size distribution, partitioning of water between gas and particle phase, onset times of freezing, freezing threshold relative humidities, aerosol chemical composition at the onset of freezing, and the number of nucleated ice crystals. The latter three parameters can directly be inferred from the experiments, the former three aid in interpreting the measurements. Sensitivity studies are carried out to address the relative importance of uncertainties of basic quantities such as temperature, H2O mixing ratio, aerosol size spectrum, and deposition coefficient of H2O molecules on ice. The ability of the numerical simulations to provide detailed explanations of the observations greatly increases confidence in attempts to model this process under real atmospheric conditions, for instance with regard to the formation of cirrus clouds or type-II polar stratospheric clouds, provided that accurate temperature and humidity measurements are available.

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    ABSTRACT: The low-temperature aerosol and cloud chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) of Forschungszentrum Karlsruhe was used to investigate the effect of sulfuric acid coating on the ice nucleation efficiency of soot aerosol particles from a spark discharge generator. The uncoated (sulfuric acid-coated) soot aerosol showed a nearly lognormal size distribution with number concentrations of 300-5000 cm-3 (2500-56,000 cm-3), count median diameters of 70-140 nm (90-200 nm), and geometric standard deviation of 1.3-1.4 (1.5-1.6). The volume fraction of the sulfuric acid coating to the total aerosol volume concentration ranged from 21 to 81%. Ice activation was investigated in dynamic expansion experiments simulating cloud cooling rates between about -0.6 and -3.5 K min-1. At temperatures between 186 and ~235 K, uncoated soot particles acted as deposition nuclei at very low ice saturation ratios between 1.1 and 1.3. Above 235 K, ice nucleation only occurred after approaching liquid saturation. Coating with sulfuric acid significantly increased the ice nucleation thresholds of soot aerosol to saturation ratios increasing from ~1.3 at 230 K to ~1.5 at 185 K. This immersion mode of freezing nucleates ice well below the thresholds for homogeneous freezing of pure sulfuric acid solution droplets measured in previous AIDA experiments. A case study indicated that in contrast to the homogeneous freezing the nucleation rate of the immersion freezing mechanism depends only weakly on relative humidity and thereby the solute concentration. These results show that it is important to know the mixing state of soot and sulfuric acid aerosol particles in order to properly assess their role in cirrus formation.
    Journal of Geophysical Research Atmospheres 01/2005; 110. · 3.44 Impact Factor
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    ABSTRACT: as such the novelty of this article is limited. The novelty, if any, lies in the well consid- ered choices made during the implementation. The implementation is described very carefully and in great detail, clearly with the purpose of later reference. This allows the reader to follow practically all the rationales, which I for most parts appreciate, even though it makes the article relatively long. I believe that in the present state, with the existing uncertainties of cirrus microphysics, the scientific community may benefit from having several existing partly redundant models focusing on different aspects of cirrus,
    Atmospheric Chemistry and Physics 01/2008; 8(1). · 4.88 Impact Factor
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    ABSTRACT: This work presents a new physically based parameterization of cirrus cloud formation for use in large-scale models which is robust, computationally efficient, and links chemical effects (e.g., water activity and water vapor deposition effects) with ice formation via homogenous freezing. The parameterization formulation is based on ascending parcel theory and provides expressions for the ice crystal size distribution and the crystal number concentration, explicitly considering the effects of aerosol size and number, updraft velocity, and deposition coefficient. The parameterization is evaluated against a detailed numerical cirrus cloud parcel model (developed during this study), the equations of which are solved using a novel Lagrangian particle-tracking scheme. Over a broad range of cirrus-forming conditions, the parameterization reproduces the results of the parcel model within a factor of 2 and with an average relative error of −15%. If numerical model simulations are used to constrain the parameterization, error further decreases to 1 ± 28%.
    Journal of Geophysical Research Atmospheres 01/2008; 113. · 3.44 Impact Factor

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