Abstract. Immersion freezing is the most relevant heterogeneous ice nucleation mechanism through which ice crystals are formed in mixed-phase clouds. In recent years, an increasing number of laboratory experiments utilizing a variety of instruments have examined immersion freezing activity of atmospherically relevant ice-nucleating particles. However, an intercomparison of these laboratory results is a difficult task because investigators have used different ice nucleation (IN) measurement methods to produce these results. A remaining challenge is to explore the sensitivity and accuracy of these techniques and to understand how the IN results are potentially influenced or biased by experimental parameters associated with these techniques.Within the framework of INUIT (Ice Nuclei Research Unit), we distributed an illite-rich sample (illite NX) as a representative surrogate for atmospheric mineral dust particles to investigators to perform immersion freezing experiments using different IN measurement methods and to obtain Published by Copernicus Publications on behalf of the European Geosciences Union. N. Hiranuma et al.: A comparison of 17 IN measurement techniquesIN data as a function of particle concentration, temperature (T ), cooling rate and nucleation time. A total of 17 measurement methods were involved in the data intercomparison. Experiments with seven instruments started with the test sample pre-suspended in water before cooling, while 10 other instruments employed water vapor condensation onto drydispersed particles followed by immersion freezing. The resulting comprehensive immersion freezing data set was evaluated using the ice nucleation active surface-site density, n s , to develop a representative n s (T ) spectrum that spans a wide temperature range (−37 • C < T < −11 • C) and covers 9 orders of magnitude in n s .In general, the 17 immersion freezing measurement techniques deviate, within a range of about 8 • C in terms of temperature, by 3 orders of magnitude with respect to n s . In addition, we show evidence that the immersion freezing efficiency expressed in n s of illite NX particles is relatively independent of droplet size, particle mass in suspension, particle size and cooling rate during freezing. A strong temperature dependence and weak time and size dependence of the immersion freezing efficiency of illite-rich clay mineral particles enabled the n s parameterization solely as a function of temperature. We also characterized the n s (T ) spectra and identified a section with a steep slope between −20 and −27 • C, where a large fraction of active sites of our test dust may trigger immersion freezing. This slope was followed by a region with a gentler slope at temperatures below −27 • C. While the agreement between different instruments was reasonable below ∼ −27 • C, there seemed to be a different trend in the temperature-dependent ice nucleation activity from the suspension and dry-dispersed particle measurements for this mineral dust, in particular at higher temperatures. For instance,...

An emerging and unsolved question is the sensitivity of cloud processes, precipitation, and climate to the atmospheric ice nucleus spectrum. This work revisits estimation of atmospheric ice‐nucleating particle concentration derived from cloud water and precipitation samples representing a wide range of geographical locations, seasons, storm systems, precipitation types, instruments, concentrations, and temperatures. Concentrations of ice‐nucleating particles are shown to vary over 10 orders of magnitude. High variability is observed in the −5°C to −12°C range which is suggested to be biologically derived nuclei whose life cycle is associated with intermittent source and efficient sink processes. The highest ever observed nucleus concentrations at −8°C are 3 orders of magnitude lower than observed ice crystal concentrations in tropical cumuli at the same temperature. The observed upper and lower limits of the nucleus spectrum provide a possible constraint on minimum enhancement factors for secondary ice formation processes.

Abstract. Recent studies have suggested that the icenucleating ability of some types of pollen is derived from non-proteinaceous macromolecules. These macromolecules may become dispersed by the rupturing of the pollen grain during wetting and drying cycles in the atmosphere. If true, this mechanism might prove to be a significant source of ice nuclei (IN) concentrations when pollen is present. Here we test this hypothesis by measuring ambient IN concentrations from the beginning to the end of the 2013 pollen season in Raleigh, North Carolina, USA. Air samples were collected using a swirling aerosol collector twice per week and the solutions were analysed for ice nuclei activity using a droplet freezing assay. Rainwater samples were collected at times when pollen grain number concentrations were near their maximum value and analysed with the drop-freezing assay to compare the potentially enhanced IN concentrations measured near the ground with IN concentrations found aloft. Ambient ice nuclei spectra, defined as the number of ice nuclei per volume of air as a function of temperature, are inferred from the aerosol collector solutions. No general trend was observed between ambient pollen grain counts and observed IN concentrations, suggesting that ice nuclei multiplication via pollen grain rupturing and subsequent release of macromolecules was not prevalent for the pollen types and meteorological conditions typically encountered in the southeastern US. A serendipitously sampled collection after a downpour provided evidence for a rain-induced IN burst with an observed IN concentration of approximately 30 per litre, a 30-fold increase over background concentrations at −20 • C. The onset temperature of freezing for these particles was approximately −12 • C, suggesting that the icenucleating particles were biological in origin.

[1] A small fraction of particles in the atmosphere can catalyze ice formation in cloud water drops through heterogeneous freezing nucleation at temperatures warmer than the homogeneous freezing temperature of approximately À38 C. The rate for heterogeneous freezing nucleation is dependent on several factors, including the type and surface area of dust that is immersed inside the drop. Although nucleation is an inherently stochastic process resulting from size fluctuations of the incipient ice germ, there is a growing body of literature that suggests that quasi-deterministic models of ice nucleation can describe laboratory experiments. Here we present new experiments and simulations that aim to better constrain theoretical models fitted to laboratory data. We collected ice nucleation data for Arizona Test Dust aerosol immersed in water using a droplet freezing assay setup that allows for the cooling rates to be changed between 10 and 0.01 K min À1 . Discrete event simulations based on a variant of the multiple-component stochastic model of heterogeneous freezing nucleation were used to simulate different experimental procedures. The nucleation properties of the dust are specified by four material-dependent parameters that accurately describe the time dependence of the freezing process. We anticipate that the combination of discrete event simulations and a spectrum of experimental procedures described here can be used to design more meaningful laboratory experiments probing ice nucleation and will aid the development of better parameterizations for use in models.

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