ALBERT

Description: The heterogeneous freezing temperatures of single binary sulfuric acid solution droplets were measured in dependency of acid concentration down to temperatures as low as -50°C. In order to avoid influence of supporting substrates on the freezing characteristics, a new technique has been developed to suspend the droplet by means of an acoustic levitator. The droplets contained immersed particles of graphite, kaolin or montmorillonite in order to study the influence of the presence of such contamination on the freezing temperature. The radii of the suspended droplets spanned the range between 0.4 and 1.1mm and the concentration of the sulfuric acid solution varied between 5 and 14 weight percent. The presence of the particles in the solution raises the freezing temperature with respect to homogeneous freezing of these solution droplets. The pure solution droplets can be supercooled up to 40 degrees below the ice-acid solution thermodynamic equilibrium curve. Depending on the concentration of sulfuric acid and the nature of the impurity the polluted droplets froze between -11°C and -35°C. The new experimental set-up, combining a deep freezer with a movable ultrasonic levitator and suitable optics, proved to be a useful approach for such investigations on individual droplets.

Description: Laboratory experiments were carried out in a vertical wind tunnel to study the retention of different atmospheric trace gases during riming. In the experiments, the rimed ice particles floated in a laminar air stream carrying a cloud of supercooled droplets with radii between 10 and 20 μm. Ice particles, dendritic ice crystals, and snow flakes with diameters between 6 mm and 1.5 cm were allowed to rime at temperatures between −5 and −12 °C where riming mainly proceeds in the atmosphere and with cloud liquid water contents between 1 and 1.5 g m−3 which are values typically found in atmospheric mixed-phase clouds. Three trace species were investigated, nitric and hydrochloric acid, and hydrogen peroxide. They were present in the supercooled liquid droplets in concentrations from 1 to 120 ppmv, i.e. similar to the concentrations measured in cloud drops. The chemical analyses of the rimed ice particles allow one to determine the trace species concentration in the ice phase. Together with the known liquid phase concentration the retention coefficients were calculated in terms of the amount of the species which remained in the ice phase after freezing. It was found that the highly soluble trace gases, nitric and hydrochloric acid, were retained nearly completely (98.6±8% and 99.7±9%, respectively) while for hydrogen peroxide a retention of 64.3±11% was determined. No influence of the riming temperature on the retention was found which can be explained by the fact that in the observed range of temperature and liquid water content, riming proceeded in the dry growth regime.

Description: Laboratory experiments were carried out in a vertical wind tunnel to study the retention of different atmospheric trace gases during riming. In the experiments, the rimed ice particles floated in a laminar air stream carrying a cloud of supercooled droplets with radii between 10 and 20 μm. Ice particles, dendritic ice crystals, and snow flakes with diameters between 6 mm and 1.5 cm were allowed to rime at temperatures between −5 and −12 °C where riming mainly proceeds in the atmosphere and with cloud liquid water contents between 1 and 1.5 g m−3 which are values typically found in atmospheric mixed phase clouds. Three trace species were investigated, nitric and hydrochloric acid, and hydrogen peroxide. They were present in the supercooled liquid droplets in concentrations from 1 to 120 ppmv, i.e. similar to the ones measured in cloud drops. The chemical analyses of the rimed ice particles allow to determine the trace species concentration in the ice phase. Together with the known liquid phase concentration the retention coefficients were calculated in terms of the amount of the species which remained in the ice phase after freezing. It was found that the highly soluble trace gases nitric and hydrochloric acid were retained nearly completely (98.6 ± 8 % and 99.7 ± 9 %, respectively) while for hydrogen peroxide a retention coefficient of 64.3 ± 11 % was determined. No influence of the riming temperature on the retention was found which can be explained by the fact that in the observed range of temperature and liquid water content riming proceeded in the dry growth regime.

Description: Based on the outcome of laboratory results, new particle-dependent parameterizations of heterogeneous freezing were derived and used to improve and extend a two-dimensional spectral microphysics scheme. They include (1) a particle-type dependent parameterization of immersion freezing using the numbers of active sites per mass, (2) a particle-type and size-resolved parameterization of contact freezing, and (3) a particle-type dependent description of deposition freezing. The modified microphysical scheme was embedded in an adiabatic air parcel model with entrainment. Sensitivity studies were performed to simulate convective situations and the impact of ice nuclei concentrations and types on ice formation. As a central diagnostic parameter the ice water fraction IWF was selected which is the relation of the ice water content to the total water content. The following parameters were varied: initial aerosol particle number size distributions, types of ice nucleating particles, strength of convection, and the fractions of potential ice nucleating particles. Single and coupled freezing processes were investigated. The results show that immersion freezing seems to be the most efficient process and, in competition with contact freezing, the dominant process. Contact freezing is constrained by the collision kernel between supercooled drops and potential ice nucleating particles and becomes relevant at temperatures lower than −25 °C. The importance of deposition freezing lies in secondary ice formation, i.e. small ice particles produced by deposition nucleation trigger the freezing of supercooled drops by collisions. Thus, a broader ice particle spectrum is generated than by immersion and contact freezing. Competition of contact and deposition freezing is negligible because of involved particle sizes. As already suggested in literature, mineral dust particles seem to be the most important ice nucleating particles. Biological particles are probably not involved in significant ice formation.

Description: The heterogeneous freezing temperatures of supercooled drops were measured by using an acoustic levitator. This technique allows to freely suspending single drops in air without electrical charges thereby avoiding any electrical influences which may affect the freezing process. Heterogeneous nucleation caused by several mineral dust particles (montmorillonite, two types of illite) was investigated in the immersion mode. Drops of 1 unit{mm} in radius were monitored by a~video camera during cooling down to −28 °C to simulate the tropospheric temperature range. The surface temperature of the drops was remotely determined with an infra-red thermometer so that the onset of freezing was indicated. For comparisons, measurements with one particle type were additionally performed in the Mainz vertical wind tunnel with drops of 340 unit{{mu}m} radius freely suspended. The data were interpreted regarding the particle surfaces immersed in the drops. Immersion freezing was observed in a~temperature range between −13 and −26 °C in dependence of particle type and surface area per drop. The results were evaluated by applying two descriptions of heterogeneous freezing, the stochastic and the singular model.

Description: The heterogeneous freezing temperatures of single binary sulphuric acid solution droplets were measured in dependency of acid concentration down to temperatures as low as −70°C. In order to avoid influence of supporting substrates on the freezing characteristics, the droplets were suspended by means of an acoustic levitator. The droplets contained immersed particles of graphite, kaolin or montmorillonite in order to study the influence of the presence of such contamination on the freezing temperature. The radii of the suspended droplets spanned the range between 0,4 and 1,1 mm and the concentration of the sulphuric acid solution varied between 5 and 25 weight percent. The presence of the particles in the solution raises the freezing temperature with respect to homogeneous freezing of these solution droplets. The pure solution droplets can be supercooled up to 40° below the ice-acid solution thermodynamic equilibrium curve. Depending on the concentration of sulphuric acid and the nature of the impurity the polluted droplets froze between −11°C and −35°C. The experimental set-up, combining a deep freezer with a movable ultrasonic levitator and suitable optics, proved to be a useful approach for such investigations on individual droplets.

Description: Based on the outcome of laboratory results, new particle-dependent parameterizations of heterogeneous freezing were derived and used to improve and extend a two-dimensional spectral microphysics scheme. They include (1) a particle-type-dependent parameterization of immersion freezing using the numbers of active sites per mass, (2) a particle-type and size-resolved parameterization of contact freezing, and (3) a particle-type-dependent description of deposition freezing. The modified microphysical scheme was embedded in an adiabatic air parcel model with entrainment. Sensitivity studies were performed to simulate convective situations and to investigate the impact of ice nuclei concentrations and types on ice formation. As a central diagnostic parameter, the ice water fraction (IWF) was selected, which is the relation of the ice water content to the total amount of water in the condensed form. The following parameters were varied: initial aerosol particle number size distributions, types of ice nucleating particles, final temperature, and the fractions of potential ice nucleating particles. Single and coupled freezing processes were investigated. The results show that immersion freezing seems to be the most efficient process. Contact freezing is constrained by the collision kernel between supercooled drops and potential ice nucleating particles. The importance of deposition freezing lies in secondary ice formation; i.e., small ice particles produced by deposition nucleation trigger the freezing of supercooled drops by collisions. Thus, a broader ice particle spectrum is generated than that by immersion and contact freezing. During coupled immersion–contact and contact–deposition freezing no competition was observed, and both processes contribute to cloud ice formation but do not impede each other. As already suggested in the literature, mineral dust particles seem to be the most important ice nucleating particles. Biological particles are probably not involved in significant ice formation. The sensitive parameters affecting cloud properties are temperature, aerosol particle composition and concentration, and particle size distribution.

Description: Three dimensional air bubble structure including size distribution, concentration and spatial distribution are important clues in identifying the growth regime of graupel and hailstone. For imaging of the bubble structure, a cryo-stage was developed to adapt to the standard setup of the SLS X04SA tomography beamline (actually replaced by the TOMCAT beamline) at the Swiss Light Source synchrotron facility to the requirements of ice particle micro-tomography. The cryo-stage setup provides for the first time 3-D-data on the individual inner pore shape delineation down to μm spatial (voxel) resolution of sub-mm small naturally as well as wind tunnel rimed graupel particles. Special care must be taken for maintaining a cooling chain between sampling and measurement. It must be kept at liquid nitrogen temperature (77 K) until measurement of the original structure at the μm spatial scale. However, even at that temperature there is no chance to preserve any ice bubble structure at sub-μm spatial resolution due to the Kelvin effect. In natural graupel grains, Y-shaped morphology of air-filled pores was found. This morphology transformed into smaller and rounded voids well-known from literature when the ice particle was annealed for as short as half an hour at 265 K and must, therefore, be regarded as artificial rather than representing the in situ pore structure. With the new synchrotron tomography approach, quantitative information on the in situ pore structure statistics within individual samples representative for a known or, thus, deduced growth mode or history can be derived, in particular if combined with airplane sampling in the troposphere at in situ growth conditions.

Description: The heterogeneous freezing temperatures of supercooled drops were measured using an acoustic levitator. This technique allows one to freely suspend single drops in the air without any wall contact. Heterogeneous nucleation by two types of illite (illite IMt1 and illite NX) and a montmorillonite sample was investigated in the immersion mode. Drops of 1 mm in radius were monitored by a video camera while cooled down to −28 °C to simulate freezing within the tropospheric temperature range. The surface temperature of the drops was contact-free, determined with an infrared thermometer; the onset of freezing was indicated by a sudden increase of the drop surface temperature. For comparison, measurements with one particle type (illite NX) were additionally performed in the Mainz vertical wind tunnel with drops of 340 μm radius freely suspended. Immersion freezing was observed in a temperature range between −13 and −26 °C as a function of particle type and particle surface area immersed in the drops. Isothermal experiments in the wind tunnel indicated that after the cooling stage freezing still proceeds, at least during the investigated time period of 30 s. The results were evaluated by applying two descriptions of heterogeneous freezing, the stochastic and the singular model. Although the wind tunnel results do not support the time-independence of the freezing process both models are applicable for comparing the results from the two experimental techniques.