Measuring systems for atmospheric ice nuclei are undergoing development anew and are beginning to meet the needs for studies of aerosol effects on ice-containing clouds. U nderstanding and predicting the formation of ice in clouds and its possible relation to the changing state of atmospheric composition (aerosols and gas phase) remain enigmatic. Such knowledge and capabilities are critical to quantifying the role of aerosols and their changing compositions on clouds, precipitation, and climate (Denman et al. 2007;Levin and Cotton 2009). This challenge is a major motivation for renewed attempts to measure ice nucleation processes in general, and to design and deploy new portable systems for measuring ice nuclei (IN), the particles that are considered the only means for initiation of the ice phase at temperatures warmer than about −36°C in the atmosphere. The fundamental desire to understand ice nucleation remains the same as when such research began in earnest more than 60 yr ago. The search to identify atmospheric ice nuclei lapsed during the 1970s-80s

Heterogeneous nucleation of ice in a supercooled water droplet induced by external contact with a dry aerosol particle has long been known to be more effective than freezing induced by the same nucleus immersed in the droplet. However, the experimental quantification of contact freezing is challenging. Here we report an experimental method to determine the temperature-dependent ice nucleation probability of size-selected aerosol particles. The method is based on the suspension of supercooled charged water droplets in a laminar flow of air containing aerosol particles as contact freezing nuclei. The rate of droplet–particle collisions is calculated numerically with account for Coulomb attraction, drag force and induced dipole interaction between charged droplet and aerosol particles. The calculation is verified by direct counting of aerosol particles collected by a levitated droplet. By repeating the experiment on individual droplets for a sufficient number of times, we are able to reproduce the statistical freezing behavior of a large ensemble of supercooled droplets and measure the average rate of freezing events. The freezing rate is equal to the product of the droplet–particle collision rate and the probability of freezing on a single contact, the latter being a function of temperature, size and composition of the contact ice nuclei. Based on these observations, we show that for the types of particles investigated so far, contact freezing is the dominating freezing mechanism on the timescale of our experiment

Charge induced changes in homogeneous freezing rates of water have been proposed to constitute a possible link between the global atmospheric electric circuit and cloud microphysics and thus climate. We report here on high precision measurements of the homogeneous nucleation rate of charged, electro-dynamically levitated single water droplets as a function of their surface charge. No evidence has been found that the homogeneous volume specific ice nucleation rate of supercooled microdroplets is influenced by surface charges in the range between +/-200 elementary charges per μm(2). It has also been suggested that filamentation in highly electrified liquids can induce freezing at temperatures well above the homogeneous freezing limit. We report here the observation of Coulomb instabilities of highly charged droplets that are accompanied with the formation and ejection of fine filaments from the liquid supercooled droplets. Down to temperatures of 240 K, which is close to the homogeneous freezing limit of uncharged water, no filamentation induced freezing has been detected. At even lower temperatures, the droplets froze before the instability was reached. These findings rule out that filamentation exerts an important influence on ice formation in supercooled water. Combining these findings, we conclude that the surface charges (even at their maximum possible density) have no significant effect on the homogeneous ice nucleation rate of supercooled cloud droplets.

Abstract. Atmospheric liquid and solid water particles are stabilized if they are coated with either negative or positive electric charge. The surface charge causes an increase of the partial pressure of water vapour close to the surface of each particle, effectively allowing the particles to remain in their condensed phase even if the environmental relative humidity drops below unity. The theory, briefly presented in this paper, predicts a zero parameter relation between surface charge density and water vapour pressure. This relation was tested in a series of Electrodynamic Balance experiments. The measurements were performed by stabilizing charged droplets of pure water near an ice-surface. We observed a divergence in radius as the temperature approached the freezing point from below. We find that the measurements confirm the theory within the experimental uncertainty. In some cases this generally overlooked effect may have impact on cloud processes and on results produced by Electrodynamic Balance experiments.

Atmospheric liquid and solid water particles are stabilized if they are coated with either negative or positive electric charge. The surface charge causes an increase of the partial pressure of water vapour close to the surface of each particle, effectively allowing the particles to remain in their condensed phase even if the environmental relative humidity drops below unity. The theory, briefly presented in this paper, predicts a zero parameter relation between surface charge density and water vapour pressure. This relation was tested in a series of Electrodynamical Balance experiments. The measurements were performed by stabilizing charged droplets of pure water near an ice-surface. We observed a divergence in radius as the temperature approached the freezing point from below. We find that the measurements confirm the theory within the experimental uncertainty. In some cases this generally overlooked effect may have impact on cloud processes and on results produced by Electrodynamical Balance experiments