Abstract:[1] Using optical microscopy, we investigated the heterogeneous nucleation of ice in aqueous (NH 4 ) 2 SO 4 -H 2 O particles containing two types of mineral dusts, kaolinite and montmorillonite. The efficacy of montmorillonite and kaolinite to nucleate ice in (NH 4 ) 2 SO 4 -H 2 O particles is similar. The difference in freezing temperatures, compared to the homogeneous freezing temperatures, is found to vary from 8 -20 K and it is larger for particles with concentrations greater than 27 wt %. Our freezing dat… Show more
“…equation 6), if the aerosol particles consist primarily of two components (e.g., submicrometer particles and supermicrometer mineral dust particles) and if the variabilities in d a,coarse and d a,fine were small. It is also important to investigate the dependence of the d a value of dust particles on their internal mixing state (whether they are coated with solution or not) because the mixing state critically affects its direct radiative effect [Ackerman and Toon, 1981] as well as its cloud microphysical properties; they would activate as cloud condensation nuclei at lower supersaturations [e.g., Takeda and Kuba, 1982] and as ice forming nuclei in the immersion-freezing mode at lower supersaturations and warmer temperatures [Zuberi et al, 2002] when they were coated with solution.…”
Section: Total Aerosol Linear Depolarization Ratiomentioning
[1] The vertical distributions of tropospheric aerosol properties were measured during the Asian dust event over central Japan (35°-36°N, 136°-137°E), using a ground-based Raman lidar and aircraft-based instruments on 23 April 1996. The lidar measured enhancements of aerosol backscattering below an altitude of 4 km and between 5 and 8 km where the total aerosol linear depolarization ratio showed peaks of 12-15% and the relative humidities were $30%. The aircraft measurements showed that the aerosol particles consisted primarily of irregularly shaped mineral dusts and sea salts with a mode radius (r m ) of $1 mm and sulfates with r m $ 0.1 mm over the measured height range of 0.6-5.5 km. Electron microscopic analyses suggest that $77% of the mineral particles were coated with a solution at 1.8 km and that the fraction of coated particles decreased with height. The aerosol backscattering coefficients (b a ), calculated from the airborne optical particle counter (OPC) data, were smaller than the lidar-derived values by $30% above 3.1 km and by $44% below that altitude. The difference was attributable to the horizontal and temporal inhomogeneities of the aerosol properties between the measurement sites and to the uncertainty in b a , particularly for the coarse particles calculated from the OPC data. The aerosol depolarization ratios (d a ) estimated from the OPC data showed the same increase as those obtained with the lidar above 4.1 km. This suggests that the proportion of backscattering by coarse particles to total particles primarily controlled the d a measured with the lidar in that region.
“…equation 6), if the aerosol particles consist primarily of two components (e.g., submicrometer particles and supermicrometer mineral dust particles) and if the variabilities in d a,coarse and d a,fine were small. It is also important to investigate the dependence of the d a value of dust particles on their internal mixing state (whether they are coated with solution or not) because the mixing state critically affects its direct radiative effect [Ackerman and Toon, 1981] as well as its cloud microphysical properties; they would activate as cloud condensation nuclei at lower supersaturations [e.g., Takeda and Kuba, 1982] and as ice forming nuclei in the immersion-freezing mode at lower supersaturations and warmer temperatures [Zuberi et al, 2002] when they were coated with solution.…”
Section: Total Aerosol Linear Depolarization Ratiomentioning
[1] The vertical distributions of tropospheric aerosol properties were measured during the Asian dust event over central Japan (35°-36°N, 136°-137°E), using a ground-based Raman lidar and aircraft-based instruments on 23 April 1996. The lidar measured enhancements of aerosol backscattering below an altitude of 4 km and between 5 and 8 km where the total aerosol linear depolarization ratio showed peaks of 12-15% and the relative humidities were $30%. The aircraft measurements showed that the aerosol particles consisted primarily of irregularly shaped mineral dusts and sea salts with a mode radius (r m ) of $1 mm and sulfates with r m $ 0.1 mm over the measured height range of 0.6-5.5 km. Electron microscopic analyses suggest that $77% of the mineral particles were coated with a solution at 1.8 km and that the fraction of coated particles decreased with height. The aerosol backscattering coefficients (b a ), calculated from the airborne optical particle counter (OPC) data, were smaller than the lidar-derived values by $30% above 3.1 km and by $44% below that altitude. The difference was attributable to the horizontal and temporal inhomogeneities of the aerosol properties between the measurement sites and to the uncertainty in b a , particularly for the coarse particles calculated from the OPC data. The aerosol depolarization ratios (d a ) estimated from the OPC data showed the same increase as those obtained with the lidar above 4.1 km. This suggests that the proportion of backscattering by coarse particles to total particles primarily controlled the d a measured with the lidar in that region.
“…Molecular dynamics simulations have contributed to shed some doubt on the validity of classical nucleation theory. Chushak and Bartell [62] and Chushak and Bartell [63] performed simulations of spontaneous phase transition in large, deeply supercooled clusters of SeF 6 . A striking result was that nucleation invariably occurred at or near the cluster's surface, despite the fact that surfaces of clusters tend to be disordered and melt at significantly lower temperatures than their cores.…”
Section: Discussionmentioning
confidence: 99%
“…Heterogeneous freezing occurs at lower supersaturation and higher temperatures than homogeneous freezing [6] [7].…”
The formation of ice in clouds can occur through primary processes, either homogeneously or heterogeneously triggered by aerosol particles called ice nuclei, as well as through secondary processes. The homogeneous ice nucleation process involves only pure water or solution droplets. Homogeneous freezing is crucial for the microphysics in the formation of high-altitude cirrus and polar stratospheric clouds, and also in the glaciation of thunderclouds, at temperatures below about 235 K. Nucleation rates in supercooled water have been measured using different experimental techniques: expansion cloud chambers, water-in-oil emulsions, levitation methods, free falling droplets, supersonic nozzles, field measurements, and molecular dynamics simulations. An important question concerns the possibility that the nucleation process in supercooled water can occur not only in the interior volume of the droplet, but even at or close to its surface. Even if there is no conclusive evidence, the majority of experimental and theoretical results suggest that the contribution of surface nucleation increases with decreasing radius of the supercooled droplets, and the surface (or sub-surface) nucleation rate is prevalent for droplets with radius lower than about 5 μm. If homogeneous freezing initiates at the droplet surface, the freezing rate should depend on the droplet size, and even a slight contamination by molecules within the surface layer could hamper the rate of the nucleation process.
“…Mineral dust aerosols are thought to play an important role as ice nuclei in mixed phase and ice clouds in the atmosphere (Zuberi et al 2002;. Evidence of Asian desert dust particles acting as effective ice nuclei at temperatures warmer than that required for homogeneous freezing was obtained from continuous flow diffusion chamber data .…”
Section: Introductionmentioning
confidence: 99%
“…In the immersion mode, all biological particles showed higher median freezing temperatures than the mineral dust particles and soot. Montmorillonite can also act as an efficient ice nucleus in immersion mode, causing aqueous (NH 4 ) 2 SO 4 -H 2 O particles to freeze at warmer temperatures (Zuberi et al 2002).…”
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