Studies on the Competition Between Homogeneous and Heterogeneous Ice Nucleation in Cirrus Formation

Cirrus ice crystals are produced heterogeneously on ice-nucleating particles (INPs) and homogeneously in supercooled liquid solution droplets. They grow by uptake of water molecules from the ice-supersaturated vapor. The precursor particles, characterized by disparate ice nucleation abilities and number concentrations, compete for available vapor during ice formation events. We investigate cirrus formation events systematically in different temperature and updraft regimes, and for different INP number concentrations and time-independent nucleation efficiencies. We consider vertical air motion variability due to mesoscale gravity waves and effects of supersaturation-dependent deposition coefficients for water molecules on ice surfaces. We analyze ice crystal properties to better understand the dynamics of competing nucleation processes

Surface modification of mineral dust particles by sulphuric acid processing: Implications for ice nucleation abilities

The ability of coated mineral dust particles to act as ice nuclei (IN) was investigated at LACIS (Leipzig Aerosol Cloud Interaction Simulator) during the FROST1- and FROST2-campaigns (Freezing of dust). Sulphuric acid was condensed on the particles which afterwards were optionally humidified, treated with ammonia vapour and/or heat. By means of aerosol mass spectrometry we found evidence that processing of mineral dust particles with sulphuric acid leads to surface modifications of the particles. These surface modifications are most likely responsible for the observed reduction of the IN activation of the particles. The observed particle mass spectra suggest that different treatments lead to different chemical reactions on the particle surface. Possible chemical reaction pathways and products are suggested and the implications on the IN efficiency of the treated dust particles are discussed

Tropical and subtropical cloud transitions in weather and climate prediction models: The GCSS/WGNE pacific cross-section intercomparison (GPCI)

International audienceA model evaluation approach is proposed in which weather and climate prediction models are analyzed along a Pacific Ocean cross section, from the stratocumulus regions off the coast of California, across the shallow convection dominated trade winds, to the deep convection regions of the ITCZ-the Global Energy and Water Cycle Experiment Cloud System Study/Working Group on Numerical Experimentation (GCSS/WGNE) Pacific Cross-Section Intercomparison (GPCI). The main goal of GPCI is to evaluate and help understand and improve the representation of tropical and subtropical cloud processes in weather and climate prediction models. In this paper, a detailed analysis of cloud regime transitions along the cross section from the subtropics to the tropics for the season June-July-August of 1998 is presented. This GPCI study confirms many of the typical weather and climate prediction model problems in the representation of clouds: underestimation of clouds in the stratocumulus regime by most models with the corresponding consequences in terms of shortwave radiation biases; overestimation of clouds by the 40-yrECMWFRe-Analysis (ERA-40) in the deep tropics (in particular) with the corresponding impact in the outgoing longwave radiation; large spread between the different models in terms of cloud cover, liquid water path and shortwave radiation; significant differences between the models in terms of vertical cross sections of cloud properties (in particular), vertical velocity, and relative humidity. An alternative analysis of cloud cover mean statistics is proposed where sharp gradients in cloud cover along the GPCI transect are taken into account. This analysis shows that the negative cloud bias of some models and ERA-40 in the stratocumulus regions [as compared to the first International Satellite Cloud Climatology Project (ISCCP)] is associated not only with lower values of cloud cover in these regimes, but also with a stratocumulus-to-cumulus transition that occurs too early along the trade wind Lagrangian trajectory. Histograms of cloud cover along the cross section differ significantly between models. Some models exhibit a quasi-bimodal structure with cloud cover being either very large (close to 100%) or very small, while other models show a more continuous transition. The ISCCP observations suggest that reality is in-between these two extreme examples. These different patterns reflect the diverse nature of the cloud, boundary layer, and convection parameterizations in the participating weather and climate prediction models. © 2011 American Meteorological Society

Homogeneous nucleation of water in synthetic air

Homogeneous nucleation rates for water vapor in synthetic air are measured by means of a Pulse-Expansion Wave Tube (PEWT). A comparison of the experimental nucleation rates with the Classical Nucleation Theory (CNT) shows that a more elaborated model is necessary to describe supercooled water nucleation at elevated pressures (10 bar). CNT is about 3 orders of magnitude off in case of our measurements. The overall trends, however, are predicted reasonably well by CNT. The size of the critical cluster (n*CNT) is predicted to be about 29 water molecules. The size of the critical cluster is obtained experimentally as well using the Nucleation Theorem. The result for water nucleation at a nucleation pressure of 10 bar and nucleation temperature of approximately 238 K is: n* = 21±1 water molecules

An OpenFOAM®-based tool for computational modeling of aerosol nucleation and transport

In the process of single-species homogeneous vapor condensation into aerosol, surface is created between liquid and vapor. The energy of formation of such surface limits the condensation of vapor from a supersaturated state. Nucleation, the mechanism of generation of embryo sites, or nuclei, on which vapor is able to condense, is an important process. Developing an understanding of this process is important, as it may lead to a considerable contribution to many engineering problems, as well as atmospheric and environmental science. In this work, we present an OpenFOAM®-based numerical simulation tool, which is capable of predicting aerosol formation using a two-moment representation of the aerosol and classical nucleation theory. We aim at developing a flexible utility, which enables researchers interested in various aerosol production-related applications to quickly study concepts like aerosol nucleation, condensation, diffusion and transport. We compare our numerical approach with the results of physical experiments, each using a laminar flow diffusion chamber (Ref. [1, 2, 3]) with different species and/or carrier gasses. A good agreement between experimental and numerical results for the aerosol droplet number density is shown

Surface modification of mineral dust particles by sulphuric acid processing: implications for ice nucleation abilities

The ability of coated mineral dust particles to act as ice nuclei (IN) was investigated at LACIS (Leipzig Aerosol Cloud Interaction Simulator) during the FROST1- and FROST2-campaigns (Freezing of dust). Sulphuric acid was condensed on the particles which afterwards were optionally humidified, treated with ammonia vapour and/or heat. By means of aerosol mass spectrometry we found evidence that processing of mineral dust particles with sulphuric acid leads to surface modifications of the particles. These surface modifications are most likely responsible for the observed reduction of the IN activation of the particles. The observed particle mass spectra suggest that different treatments lead to different chemical reactions on the particle surface. Possible chemical reaction pathways and products are suggested and the implications on the IN efficiency of the treated dust particles are discussed