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- Author or Editor: Paul J. DeMott x
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Abstract
The activities of nearly monodisperse soot particles as ice nuclei at temperatures below −20°C were examined in a short series of experiments. A continuous slow expansion cloud chamber was used to cause cloud formation and growth on soot during simulations of adiabatic cooling by expansion. Soot was generated using an acetylene burner operating near the sooting limit. Activity as ice nuclei was measured as clouds cooled to the apparent homogeneous-freezing temperatures of the cloud droplets. Immersion-freezing nucleation appears to be a particularly dominant heterogeneous mode for these particles. The preliminary results suggest that activity by immersion-freezing increases with particle size.
Abstract
The activities of nearly monodisperse soot particles as ice nuclei at temperatures below −20°C were examined in a short series of experiments. A continuous slow expansion cloud chamber was used to cause cloud formation and growth on soot during simulations of adiabatic cooling by expansion. Soot was generated using an acetylene burner operating near the sooting limit. Activity as ice nuclei was measured as clouds cooled to the apparent homogeneous-freezing temperatures of the cloud droplets. Immersion-freezing nucleation appears to be a particularly dominant heterogeneous mode for these particles. The preliminary results suggest that activity by immersion-freezing increases with particle size.
Abstract
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Abstract
A 1.2 m3 continuous slow-expansion cloud chamber was used to simulate natural, liquid cloud formation on soluble cloud condensation nuclei (CCN). Droplet freezing was observed during continued simulated adiabatic ascent and cooling to −40°C. Sharply increasing ice nucleation rates were observed between −34° and −39°C, independent of the chemical composition of three CCN used. From the experimental data, nucleation rates are estimated assuming a homogeneous-freezing mechanism. It is concluded that homogeneous-freezing was observed. The results are compared to other laboratory and field studies. These results compare most closely with values calculated from data taken in real clouds and should be relevant to ice formation in cirrus clouds.
Abstract
A 1.2 m3 continuous slow-expansion cloud chamber was used to simulate natural, liquid cloud formation on soluble cloud condensation nuclei (CCN). Droplet freezing was observed during continued simulated adiabatic ascent and cooling to −40°C. Sharply increasing ice nucleation rates were observed between −34° and −39°C, independent of the chemical composition of three CCN used. From the experimental data, nucleation rates are estimated assuming a homogeneous-freezing mechanism. It is concluded that homogeneous-freezing was observed. The results are compared to other laboratory and field studies. These results compare most closely with values calculated from data taken in real clouds and should be relevant to ice formation in cirrus clouds.
Abstract
Several strains of plant pathogenic bacteria, Erwinia carotovora carotovora and E. carotovora atroseptica, were observed to be active as cloud condensation nuclei (CCN). The CCN supersaturation spectra of bacterial aerosols were measured in the laboratory and compared to the activity of ammonium sulfate. Approximately 25%–30% of the aerosolized bacterial cells activated droplets at 1% water supersaturation compared to 80% activation of the ammonium sulfate aerosol. Physical and numerical simulations of cloud droplet activation and growth on bacteria were also performed. Both simulations predict that aerosolized bacteria will be incorporated into cloud droplets during cloud formation. Results strongly support the hypothesis that significant numbers of the tested bacterial strains are actively involved in atmospheric cloud formation and precipitation processes following natural aerosolization and vertical transport to cloud levels.
Abstract
Several strains of plant pathogenic bacteria, Erwinia carotovora carotovora and E. carotovora atroseptica, were observed to be active as cloud condensation nuclei (CCN). The CCN supersaturation spectra of bacterial aerosols were measured in the laboratory and compared to the activity of ammonium sulfate. Approximately 25%–30% of the aerosolized bacterial cells activated droplets at 1% water supersaturation compared to 80% activation of the ammonium sulfate aerosol. Physical and numerical simulations of cloud droplet activation and growth on bacteria were also performed. Both simulations predict that aerosolized bacteria will be incorporated into cloud droplets during cloud formation. Results strongly support the hypothesis that significant numbers of the tested bacterial strains are actively involved in atmospheric cloud formation and precipitation processes following natural aerosolization and vertical transport to cloud levels.
Abstract
A novel, flexible framework is proposed for parameterizing the heterogeneous nucleation of ice within clouds. It has empirically derived dependencies on the chemistry and surface area of multiple species of ice nucleus (IN) aerosols. Effects from variability in mean size, spectral width, and mass loading of aerosols are represented via their influences on surface area. The parameterization is intended for application in large-scale atmospheric and cloud models that can predict 1) the supersaturation of water vapor, which requires a representation of vertical velocity on the cloud scale, and 2) concentrations of a variety of insoluble aerosol species.
Observational data constraining the parameterization are principally from coincident field studies of IN activity and insoluble aerosol in the troposphere. The continuous flow diffusion chamber (CFDC) was deployed. Aerosol species are grouped by the parameterization into three basic types: dust and metallic compounds, inorganic black carbon, and insoluble organic aerosols.
Further field observations inform the partitioning of measured IN concentrations among these basic groups of aerosol. The scarcity of heterogeneous nucleation, observed at humidities well below water saturation for warm subzero temperatures, is represented. Conventional and inside-out contact nucleation by IN is treated with a constant shift of their freezing temperatures.
The empirical parameterization is described and compared with available field and laboratory observations and other schemes. Alternative schemes differ by up to five orders of magnitude in their freezing fractions (−30°C). New knowledge from future observational advances may be easily assimilated into the scheme’s framework. The essence of this versatile framework is the use of data concerning atmospheric IN sampled directly from the troposphere.
Abstract
A novel, flexible framework is proposed for parameterizing the heterogeneous nucleation of ice within clouds. It has empirically derived dependencies on the chemistry and surface area of multiple species of ice nucleus (IN) aerosols. Effects from variability in mean size, spectral width, and mass loading of aerosols are represented via their influences on surface area. The parameterization is intended for application in large-scale atmospheric and cloud models that can predict 1) the supersaturation of water vapor, which requires a representation of vertical velocity on the cloud scale, and 2) concentrations of a variety of insoluble aerosol species.
Observational data constraining the parameterization are principally from coincident field studies of IN activity and insoluble aerosol in the troposphere. The continuous flow diffusion chamber (CFDC) was deployed. Aerosol species are grouped by the parameterization into three basic types: dust and metallic compounds, inorganic black carbon, and insoluble organic aerosols.
Further field observations inform the partitioning of measured IN concentrations among these basic groups of aerosol. The scarcity of heterogeneous nucleation, observed at humidities well below water saturation for warm subzero temperatures, is represented. Conventional and inside-out contact nucleation by IN is treated with a constant shift of their freezing temperatures.
The empirical parameterization is described and compared with available field and laboratory observations and other schemes. Alternative schemes differ by up to five orders of magnitude in their freezing fractions (−30°C). New knowledge from future observational advances may be easily assimilated into the scheme’s framework. The essence of this versatile framework is the use of data concerning atmospheric IN sampled directly from the troposphere.
Abstract
Two new primary ice-nucleation parameterizations are examined in the Regional Atmospheric Modeling System (RAMS) cloud model via sensitivity tests on a wintertime precipitation event in the Sierra Nevada region. A model combining the effects of deposition and condensation-freezing nucleation is formulated based on data obtained from continuous-flow diffusion chambers. The data indicate an exponential variation of ice-nuclei concentrations with ice supersaturation reasonably independent of temperatures between −7° and −20°C. Predicted ice concentrations from these measurements exceed values predicted by the widely used temperatures dependent Fletcher approximation by as much as one order of magnitude at temperatures warmer than −20°C. A contact-freezing nucleation model is also formulated based on laboratory data gathered by various authors using techniques that isolated this nucleation mode. Predicted contact nuclei concentrations based on the newer measurements are as much as three orders of magnitude less than values estimated by Young's model, which has been widely used for predicted schemes.
Simulations of the orographic precipitation event over the Sierra Nevada indicate that the pristine ice fields are very sensitive to the changes in the ice-nucleation formulation, with the pristine ice field resulting from the new formulation comparing much better to the observed magnitudes and structure from the case study. Deposition-condensation-freezing nucleation dominates contact-freezing nucleation in the new scheme, except in the downward branch of the mountain wave, where contact freezing dominates in the evaporating cloud. Secondary ice production is more dominant at warm temperatures in the new scheme, producing more pristine ice crystals over the barrier. The old contact-freezing nucleation scheme overpredicts pristine ice-crystal concentrations, which depletes cloud water available for secondary ice production. The effect of the new parameterizations on the precipitating hydrometeors is substantial with nearly a 10% increase in precipitation across the domain. Graupel precipitation increased dramatically due to more cloud water available with the new scheme.
Abstract
Two new primary ice-nucleation parameterizations are examined in the Regional Atmospheric Modeling System (RAMS) cloud model via sensitivity tests on a wintertime precipitation event in the Sierra Nevada region. A model combining the effects of deposition and condensation-freezing nucleation is formulated based on data obtained from continuous-flow diffusion chambers. The data indicate an exponential variation of ice-nuclei concentrations with ice supersaturation reasonably independent of temperatures between −7° and −20°C. Predicted ice concentrations from these measurements exceed values predicted by the widely used temperatures dependent Fletcher approximation by as much as one order of magnitude at temperatures warmer than −20°C. A contact-freezing nucleation model is also formulated based on laboratory data gathered by various authors using techniques that isolated this nucleation mode. Predicted contact nuclei concentrations based on the newer measurements are as much as three orders of magnitude less than values estimated by Young's model, which has been widely used for predicted schemes.
Simulations of the orographic precipitation event over the Sierra Nevada indicate that the pristine ice fields are very sensitive to the changes in the ice-nucleation formulation, with the pristine ice field resulting from the new formulation comparing much better to the observed magnitudes and structure from the case study. Deposition-condensation-freezing nucleation dominates contact-freezing nucleation in the new scheme, except in the downward branch of the mountain wave, where contact freezing dominates in the evaporating cloud. Secondary ice production is more dominant at warm temperatures in the new scheme, producing more pristine ice crystals over the barrier. The old contact-freezing nucleation scheme overpredicts pristine ice-crystal concentrations, which depletes cloud water available for secondary ice production. The effect of the new parameterizations on the precipitating hydrometeors is substantial with nearly a 10% increase in precipitation across the domain. Graupel precipitation increased dramatically due to more cloud water available with the new scheme.
Abstract
Mathematical and experimental errors cast doubt on the ice nucleus activity spectrum of falling dry ice pellets as reported by Fukuta et al. (1971). Preliminary laboratory studies have established that ice embryos or small ice crystals will survive at ice saturation for periods up to 15 min in the Colorado State University Isothermal Cloud Chamber following dry ice seeding. These facts suggest that a re-evaluation be made of the methodology, amounts used, and the effects expected from dry ice seeding of natural clouds.
Abstract
Mathematical and experimental errors cast doubt on the ice nucleus activity spectrum of falling dry ice pellets as reported by Fukuta et al. (1971). Preliminary laboratory studies have established that ice embryos or small ice crystals will survive at ice saturation for periods up to 15 min in the Colorado State University Isothermal Cloud Chamber following dry ice seeding. These facts suggest that a re-evaluation be made of the methodology, amounts used, and the effects expected from dry ice seeding of natural clouds.
Abstract
Chemical kinetic theory and methodology is applied to examine the ice nucleating properties of silver iodide (AgI) and silver iodide-silver chloride (AgI-AgCl) aerosols in a large cloud chamber held at water saturation. This approach uses temporal data on ice crystals formation with changes in key nucleation parameters such as temperature, water vapor concentration and droplet concentrations. The inter-relationships between ice nucleation effectiveness, nucleation mechanisms, nuclei chemical and physical properties and the rate of appearance of ice crystals can be deduced. The theory and methodology can be applied to atmospheric experimentation.
Ice nucleation effectiveness increases of up to three orders of magnitude over that of AgI aerosols can be achieved with AgI-AgCl solid solution aerosols. Both aerosols are shown to form ice crystals by predominantly contact nucleation at temperatures of −16°C and warmer. Nucleation of the ice phase following collision is identified as a very rapid process, so that the rate of appearance of ice crystals is controlled by the much slower transport rate of nuclei to cloud droplets. The higher efficiency of AgI-AgCl nuclei with respect to the standard AgI nuclei is attributed to an improvement in the relative rates of nucleation versus deactivation or solution following collision of the nuclei with cloud droplets. This increase is most probably due to epitaxy and/or surface “active site” improvements. At a temperature of −20°C, all tested aerosols formed ice crystals by a combination of contact nucleation and deposition nucleation. The percentage of ice crystals formed by deposition correlated well with a minimum particle size of 500 Å for an appreciable deposition rate.
Abstract
Chemical kinetic theory and methodology is applied to examine the ice nucleating properties of silver iodide (AgI) and silver iodide-silver chloride (AgI-AgCl) aerosols in a large cloud chamber held at water saturation. This approach uses temporal data on ice crystals formation with changes in key nucleation parameters such as temperature, water vapor concentration and droplet concentrations. The inter-relationships between ice nucleation effectiveness, nucleation mechanisms, nuclei chemical and physical properties and the rate of appearance of ice crystals can be deduced. The theory and methodology can be applied to atmospheric experimentation.
Ice nucleation effectiveness increases of up to three orders of magnitude over that of AgI aerosols can be achieved with AgI-AgCl solid solution aerosols. Both aerosols are shown to form ice crystals by predominantly contact nucleation at temperatures of −16°C and warmer. Nucleation of the ice phase following collision is identified as a very rapid process, so that the rate of appearance of ice crystals is controlled by the much slower transport rate of nuclei to cloud droplets. The higher efficiency of AgI-AgCl nuclei with respect to the standard AgI nuclei is attributed to an improvement in the relative rates of nucleation versus deactivation or solution following collision of the nuclei with cloud droplets. This increase is most probably due to epitaxy and/or surface “active site” improvements. At a temperature of −20°C, all tested aerosols formed ice crystals by a combination of contact nucleation and deposition nucleation. The percentage of ice crystals formed by deposition correlated well with a minimum particle size of 500 Å for an appreciable deposition rate.
Abstract
An effort to improve descriptions of ice initiation processes of relevance to cirrus clouds for use in regional-scale numerical cloud models with bulk microphysical schemes is described. This is approached by deriving practical parameterizations of the process of ice initiation by homogeneous freezing of cloud and haze (CCN) particles in the atmosphere. The homogeneous freezing formulations may be used with generalized distributions of cloud water and CCN (pure ammonium sulfate assumed). Numerical cloud model sensitivity experiments were made using a microphysical parcel model and a mososcale cloud model to investigate the impact of the homogeneous freezing process and heterogeneous ice nucleation processes on the formation and makeup of cirrus clouds. These studies point out the critical nature of assumptions made regarding the abundance and character of heterogeneous ice nuclei (IN) present in the upper troposphere. Conclusions regarding the sources of ice crystals in cirrus clouds and the potential impact of human activities on these populations must await further measurements of CCN and particularly IN in upper-tropospheric and lower-stratospheric regions.
Abstract
An effort to improve descriptions of ice initiation processes of relevance to cirrus clouds for use in regional-scale numerical cloud models with bulk microphysical schemes is described. This is approached by deriving practical parameterizations of the process of ice initiation by homogeneous freezing of cloud and haze (CCN) particles in the atmosphere. The homogeneous freezing formulations may be used with generalized distributions of cloud water and CCN (pure ammonium sulfate assumed). Numerical cloud model sensitivity experiments were made using a microphysical parcel model and a mososcale cloud model to investigate the impact of the homogeneous freezing process and heterogeneous ice nucleation processes on the formation and makeup of cirrus clouds. These studies point out the critical nature of assumptions made regarding the abundance and character of heterogeneous ice nuclei (IN) present in the upper troposphere. Conclusions regarding the sources of ice crystals in cirrus clouds and the potential impact of human activities on these populations must await further measurements of CCN and particularly IN in upper-tropospheric and lower-stratospheric regions.
Abstract
Ice initiation by specific cloud seeding aerosols, quantified in laboratory studies, has been formulated for use in mesoscale numerical cloud models. This detailed approach, which explicitly represents artificial ice nuclei activation, is unique for mesoscale simulators of cloud seeding. This new scheme was applied in the simulation of an orographic precipitation event seeded with the specific aerosols on 18 December 1986 from the Sierra Cooperative Pilot Project using the Regional Atmospheric Modeling System (RAMS). Total ice concentrations formed following seeding agreed well with observations. RAMS's three-dimensional results showed that the new seeding parameterization impacted the microphysical fields producing increased pristine ice crystal, aggregate, and graupel mass downstream of the seeded regions. Pristine ice concentration also increased as much as an order of magnitude in some locations due to seeding. Precipitation augmentation due to the seeding was 0.1–0.7 mm, similar to values inferred from the observations. Simulated precipitation enhancement occurred due to increased precipitation efficiency since no large precipitation deficits occurred in the simulation. These maxima were collocated with regions of supercooled liquid water where nucleation by man-made ice nucleus aerosols was optimized.
Abstract
Ice initiation by specific cloud seeding aerosols, quantified in laboratory studies, has been formulated for use in mesoscale numerical cloud models. This detailed approach, which explicitly represents artificial ice nuclei activation, is unique for mesoscale simulators of cloud seeding. This new scheme was applied in the simulation of an orographic precipitation event seeded with the specific aerosols on 18 December 1986 from the Sierra Cooperative Pilot Project using the Regional Atmospheric Modeling System (RAMS). Total ice concentrations formed following seeding agreed well with observations. RAMS's three-dimensional results showed that the new seeding parameterization impacted the microphysical fields producing increased pristine ice crystal, aggregate, and graupel mass downstream of the seeded regions. Pristine ice concentration also increased as much as an order of magnitude in some locations due to seeding. Precipitation augmentation due to the seeding was 0.1–0.7 mm, similar to values inferred from the observations. Simulated precipitation enhancement occurred due to increased precipitation efficiency since no large precipitation deficits occurred in the simulation. These maxima were collocated with regions of supercooled liquid water where nucleation by man-made ice nucleus aerosols was optimized.
