The Portable Ice Nucleation Chamber 2 (PINCii) is a newly developed continuous flow diffusion chamber (CFDC) for measuring ice nucleating particles (INPs). PINCii is a vertically oriented parallel-plate CFDC that has been engineered to improve upon the limitations of previous generations of CFDCs. This work presents a detailed description of the PINCii instrument and the upgrades that make it unique compared with other operational CFDCs. The PINCii design offers several possibilities for improved INP measurements. Notably, a specific icing procedure results in low background particle counts, which demonstrates the potential for PINCii to measure INPs at low concentrations (<10 L−1). High-spatial-resolution wall-temperature mapping enables the identification of temperature inhomogeneities on the chamber walls. This feature is used to introduce and discuss a new method for analyzing CFDC data based on the most extreme lamina conditions present within the chamber, which represent conditions most likely to trigger ice nucleation. A temperature gradient can be maintained throughout the evaporation section in addition to the main chamber, which enables PINCii to be used to study droplet activation processes or to extend ice crystal growth. A series of both liquid droplet activation and ice nucleation experiments were conducted at temperature and saturation conditions that span the spectrum of PINCii's operational conditions (-50≤ temperature ≤-15 ∘C and 100 ≤ relative humidity with respect to ice ≤160 %) to demonstrate the instrument's capabilities. In addition, typical sources of uncertainty in CFDCs, including particle background, particle loss, and variations in aerosol lamina temperature and relative humidity, are quantified and discussed for PINCii.

Ice nucleating particles (INPs) in the atmosphere are responsible for glaciating cloud droplets between 237 and 273 K. Different mechanisms of heterogeneous ice nucleation can compete under mixed-phase cloud conditions. Contact freezing is considered relevant because higher ice nucleation temperatures than for immersion freezing for the same INPs were observed. It has limitations because its efficiency depends on the number of collisions between cloud droplets and INPs. To date, direct comparisons of contact and immersion freezing with the same INP, for similar residence times and concentrations, are lacking. This study compares immersion and contact freezing efficiencies of three different INPs. The contact freezing data were obtained with the ETH CoLlision Ice Nucleation CHamber (CLINCH) using 80 µm diameter droplets, which can interact with INPs for residence times of 2 and 4 s in the chamber. The contact freezing efficiency was calculated by estimating the number of collisions between droplets and particles. Theoretical formulations of collision efficiencies gave too high freezing efficiencies for all investigated INPs, namely AgI particles with 200 nm electrical mobility diameter, 400 and 800 nm diameter Arizona Test Dust (ATD) and kaolinite particles. Comparison of freezing efficiencies by contact and immersion freezing is therefore limited by the accuracy of collision efficiencies. The concentration of particles was 1000 cm−3 for ATD and kaolinite and 500, 1000, 2000 and 5000 cm−3 for AgI. For concentrations < 5000 cm−3, the droplets collect only one particle on average during their time in the chamber. For ATD and kaolinite particles, contact freezing efficiencies at 2 s residence time were smaller than at 4 s, which is in disagreement with a collisional contact freezing process but in accordance with immersion freezing or adhesion freezing. With “adhesion freezing”, we refer to a contact nucleation process that is enhanced compared to immersion freezing due to the position of the INP on the droplet, and we discriminate it from collisional contact freezing, which assumes an enhancement due to the collision of the particle with the droplet. For best comparison with contact freezing results, immersion freezing experiments of the same INPs were performed with the continuous flow diffusion chamber Immersion Mode Cooling chAmber–Zurich Ice Nucleation Chamber (IMCA–ZINC) for a 3 s residence time. In IMCA–ZINC, each INP is activated into a droplet in IMCA and provides its surface for ice nucleation in the ZINC chamber. The comparison of contact and immersion freezing results did not confirm a general enhancement of freezing efficiency for contact compared with immersion freezing experiments. For AgI particles the onset of heterogeneous freezing in CLINCH was even shifted to lower temperatures compared with IMCA–ZINC. For ATD, freezing efficiencies for contact and immersion freezing experiments were similar. For kaolinite particles, contact freezing became detectable at higher temperatures than immersion freezing. Using contact angle information between water and the INP, it is discussed how the position of the INP in or on the droplets may influence its ice nucleation activity.

The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nucleating particle (INP) counter manufactured by Droplet Measurement Technologies in Boulder, CO. The SPIN is a continuous flow diffusion chamber with parallel plate geometry based on the Zurich Ice Nucleation Chamber and the Portable Ice Nucleation Chamber. This study presents a standard description for using the SPIN instrument and also highlights methods to analyze measurements in more advanced ways. It characterizes and describes the behavior of the SPIN chamber, reports data from laboratory measurements, and quantifies uncertainties associated with the measurements. Experiments with ammonium sulfate are used to investigate homogeneous freezing of deliquesced haze droplets and droplet breakthrough. Experiments with kaolinite, NX illite, and silver iodide are used to investigate heterogeneous ice nucleation. SPIN nucleation results are compared to those from the literature. A machine learning approach for analyzing depolarization data from the SPIN optical particle counter is also presented (as an advanced use). Overall, we report that the SPIN is able to reproduce previous INP counter measurements.

Interactions of atmospheric aerosols with clouds influence cloud properties and modify the aerosol life cycle. Aerosol particles act as cloud condensation nuclei and ice nucleating particles or become incorporated into cloud droplets by scavenging. For an accurate description of aerosol scavenging and ice nucleation in contact mode, collision efficiency between droplets and aerosol particles needs to be known. This study derives the collision rate from experimental contact freezing data obtained with the ETH CoLlision Ice Nucleation CHamber (CLINCH). Freely falling 80 μm diameter water droplets are exposed to an aerosol consisting of 200 and 400 nm diameter silver iodide particles of concentrations from 500 to 5000 and 500 to 2000 cm−3, respectively, which act as ice nucleating particles in contact mode. The experimental data used to derive collision efficiency are in a temperature range of 238–245 K, where each collision of silver iodide particles with droplets can be assumed to result in the freezing of the droplet. An upper and lower limit of collision efficiency is also estimated for 800 nm diameter kaolinite particles. The chamber is kept at ice saturation at a temperature range of 236 to 261 K, leading to the slow evaporation of water droplets giving rise to thermophoresis and diffusiophoresis. Droplets and particles bear charges inducing electrophoresis. The experimentally derived collision efficiency values of 0.13, 0.07 and 0.047–0.11 for 200, 400 and 800 nm particles are around 1 order of magnitude higher than theoretical formulations which include Brownian diffusion, impaction, interception, thermophoretic, diffusiophoretic and electric forces. This discrepancy is most probably due to uncertainties and inaccuracies in the description of thermophoretic and diffusiophoretic processes acting together. This is, to the authors' knowledge, the first data set of collision efficiencies acquired below 273 K. More such experiments with different droplet and particle diameters are needed to improve our understanding of collision processes acting together.

Introduction Conclusions References

Abstract. The climate in the Arctic is changing faster than anywhere else on earth. Poorly understood feedback processes relating to Arctic clouds and aerosol–cloud interactions contribute to a poor understanding of the present changes in the Arctic climate system, and also to a large spread in projections of future climate in the Arctic. The problem is exacerbated by the paucity of research-quality observations in the central Arctic. Improved formulations in climate models require such observations, which can only come from measurements in situ in this difficult-to-reach region with logistically demanding environmental conditions. The Arctic Summer Cloud Ocean Study (ASCOS) was the most extensive central Arctic Ocean expedition with an atmospheric focus during the International Polar Year (IPY) 2007–2008. ASCOS focused on the study of the formation and life cycle of low-level Arctic clouds. ASCOS departed from Longyearbyen on Svalbard on 2 August and returned on 9 September 2008. In transit into and out of the pack ice, four short research stations were undertaken in the Fram Strait: two in open water and two in the marginal ice zone. After traversing the pack ice northward, an ice camp was set up on 12 August at 87°21' N, 01°29' W and remained in operation through 1 September, drifting with the ice. During this time, extensive measurements were taken of atmospheric gas and particle chemistry and physics, mesoscale and boundary-layer meteorology, marine biology and chemistry, and upper ocean physics. ASCOS provides a unique interdisciplinary data set for development and testing of new hypotheses on cloud processes, their interactions with the sea ice and ocean and associated physical, chemical, and biological processes and interactions. For example, the first-ever quantitative observation of bubbles in Arctic leads, combined with the unique discovery of marine organic material, polymer gels with an origin in the ocean, inside cloud droplets suggests the possibility of primary marine organically derived cloud condensation nuclei in Arctic stratocumulus clouds. Direct observations of surface fluxes of aerosols could, however, not explain observed variability in aerosol concentrations, and the balance between local and remote aerosols sources remains open. Lack of cloud condensation nuclei (CCN) was at times a controlling factor in low-level cloud formation, and hence for the impact of clouds on the surface energy budget. ASCOS provided detailed measurements of the surface energy balance from late summer melt into the initial autumn freeze-up, and documented the effects of clouds and storms on the surface energy balance during this transition. In addition to such process-level studies, the unique, independent ASCOS data set can and is being used for validation of satellite retrievals, operational models, and reanalysis data sets.

This manuscript compiles both theoretical and experimental information on contact freezing with the aim to better understand this potentially important but still not well quantified heterogeneous freezing mode. There is no complete theory that describes contact freezing and how the energy barrier has to be overcome to nucleate an ice crystal by contact freezing. Experiments on contact freezing conducted using the cold plate technique indicate that it can initiate ice formation at warmer temperatures than immersion freezing. Additionally, a qualitative difference in the freezing temperatures between contact and immersion freezing has been found using different instrumentation and different ice nuclei. There is a lack of data on collision rates in most of the reported data, which inhibits a quantitative calculation of the freezing efficiencies. Thus, new or modified instrumentation to study contact nucleation in the laboratory and in the field are needed to identify the conditions at which contact nucleation could occur in the atmosphere. Important questions concerning contact freezing and its potential role for ice cloud formation and climate are also summarized.

Measurements of the microphysical properties of mixed-phase clouds with high spatial resolution are important to understand the processes inside these clouds. This work describes the design and characterization of the newly developed ground-based field instrument HOLIMO II (HOLographic Imager for Microscopic Objects II). HOLIMO II uses digital in-line holography to in situ image cloud particles in a well-defined sample volume. By an automated algorithm, two-dimensional images of single cloud particles between 6 and 250 μm in diameter are obtained and the size spectrum, the concentration and water content of clouds are calculated. By testing the sizing algorithm with monosized beads a systematic overestimation near the resolution limit was found, which has been used to correct the measurements. Field measurements from the high altitude research station Jungfraujoch, Switzerland, are presented. The measured number size distributions are in good agreement with parallel measurements by a fog monitor (FM-100, DMT, Boulder USA). The field data shows that HOLIMO II is capable of measuring the number size distribution with a high spatial resolution and determines ice crystal shape, thus providing a method of quantifying variations in microphysical properties. A case study over a period of 8 h has been analyzed, exploring the transition from a liquid to a mixed-phase cloud, which is the longest observation of a cloud with a holographic device. During the measurement period, the cloud does not completely glaciate, contradicting earlier assumptions of the dominance of the Wegener–Bergeron–Findeisen (WBF) process.

The immersion mode ice nucleation efficiency of clay minerals and biological aerosols has been investigated using the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber. Both monodisperse and polydisperse populations of (1) various clay dust samples as well as (2) Snomax (R) (a proxy for bacterial ice nucleators) and (3) hematite are examined in the temperature range between -4 degrees C and -35 degrees C. The temperature dependence of ice formation inferred by the INAS (Ice Nucleation Active Surface-Site) density is investigated and discussed as a function of cooling rate and by comparing to predicted nucleation rates (i. e., classical nucleation theory with theta-probability density function nucleation scheme). To date, we observe that maintaining constant AIDA temperature does not trigger any new ice formation during the immersion freezing experiments with clay dust samples and Snomax (R), implying strong temperature dependency (and weak time dependency) within our time scales and conditions of experiments. Ice residuals collected through a newly developed PCVI (Pumped Counter-flow Virtual Impactor) with the 50% cut size diameter of 10 to 20 mu m have also been examined by electron microscope analyses to seek the chemical and physical identity of ice nuclei in clay minerals. In addition to the AIDA results, complementary measurements with mobile ice nucleation counters are also presented.

Deposition and immersion mode ice nucleation studies of kaolinite (Ka) and Arizona Test Dust (ATD) particles exposed to ozone at 430 ppbv, 1.4 and 4.3 ppmv for approximately 2 hours in a stainless steel aerosol tank are presented. The polydisperse particles used have a mode mobility diameter of 800 nm for Ka and 400 nm for ATD. The portable ice nucleation chamber (PINC) and immersion chamber (IMCA-ZINC) were used to study deposition and immersion mode ice nucleation respectively. Both instruments sampled through a particle impactor with a diameter cut-off size of 1 mu m. Preliminary results indicate that ice nucleation can be enhanced or inhibited depending on ozone concentration used for the ageing process with higher concentrations suppressing ice nucleation in both immersion and deposition modes. Additionally, Ka and ATD respond differently to the ageing process and to the different modes of ice nucleation. Ozone surface coverage and initial uptake coefficients are presented for the low exposure studies to explain the ice nucleation behavior observed. Ice Active Surface Site Densities (IASSD) are presented as a means of comparison and parameterization of the data to predict potential atmospheric ice nuclei (IN) concentrations.

Ice nucleation in the atmosphere is central to the understanding the microphysical properties of mixed-phase and cirrus clouds. Ambient conditions such as temperature (T) and relative humidity (RH), as well as aerosol properties such as chemical composition and mixing state play an important role in predicting ice formation in the troposphere. Previous field studies have reported the absence of sulfate and organic compounds on mineral dust ice crystal residuals sampled at mountain top stations or aircraft based measurements despite the long-range transport mineral dust is subjected to. We present laboratory studies of ice nucleation for immersion and deposition mode on ozone aged mineral dust particles for 233 < T < 263 K. Heterogeneous ice nucleation of untreated kaolinite (Ka) and Arizona Test Dust (ATD) particles is compared to corresponding aged particles that are subjected to ozone concentrations of 0.4–4.3 ppmv in a stainless steel aerosol tank. The portable ice nucleation counter (PINC) and immersion chamber combined with the Zurich ice nucleation chamber (IMCA-ZINC) are used to conduct deposition and immersion mode measurements, respectively. Ice active fractions as well as ice active surface site densities (ns) are reported and observed to increase as a function of decreasing temperature. We present first results that demonstrate enhancement of the ice nucleation ability of aged mineral dust particles in both the deposition and immersion mode due to ageing. We also present the first results to show a suppression of heterogeneous ice nucleation activity without the condensation of a coating of (in)organic material. In immersion mode, low ozone exposed Ka particles showed enhanced ice activity requiring a median freezing temperature of 1.5 K warmer than that of untreated Ka, whereas high ozone exposed ATD particles showed suppressed ice nucleation requiring a median freezing temperature of 3 K colder than that of untreated ATD. In deposition mode, low exposure Ka had ice active fractions of an order of magnitude higher than untreated Ka, whereas high ozone exposed ATD had ice active fractions up to a factor of 4 lower than untreated ATD. From our results, we derive and present parameterizations in terms of ns(T) that can be used in models to predict ice nuclei concentrations based on available aerosol surface area.

Abstract. A measurement campaign (IMBALANCE) conducted in 2009 was aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC) but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro without emission aftertreatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC) at three nominal temperatures, −30 °C, −35 °C and −40 °C. Freshly emitted diesel particles showed ice formation only at −40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi) and 92% relative humidity with respect to water (RHw), and photochemical ageing did not play a role in modifying their ice nucleation behaviour. Only one diesel experiment where α-pinene was added for the ageing process, showed an ice nucleation enhancement at −35 °C. Wood burning particles also act as ice nuclei (IN) at −40 °C in the deposition mode at the same conditions as for diesel particles and photochemical ageing also did not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at −35 °C whereas no ice nucleation was observed at −30 °C. Photochemical ageing did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below −40 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical ageing on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.

To identify the temperature and humidity conditions at which different ice nucleation mechanisms are active, the authors conducted experiments on 200-, 400-, and 800-nm size-selected kaolinite particles, exposing them to temperatures between 218 and 258 K and relative humidities with respect to ice (RHi) between 100% and 180%, including the typical conditions for cirrus and mixed-phase-cloud formation. Measurements of the ice active particle fraction as a function of temperature and relative humidity with respect to ice are reported. The authors find enhanced activated fractions when water saturation is reached at mixed-phase-cloud temperatures between 235 and 241 K and a distinct increase in the activated fraction below 235 K at conditions below water saturation. To provide a functional description of the observed ice nucleation mechanisms, the experimental results are analyzed by two different particle-surface models within the framework of classical nucleation theory. Describing the ice nucleation activity of kaolinite particles by assuming deposition nucleation to be the governing mechanism below water saturation was found to be inadequate to represent the experimental data in the whole temperature range investigated. The observed increase in the activated fraction below water saturation and temperatures below 235 K corroborate the assumption that an appreciable amount of adsorbed or capillary condensed water is present on kaolinite particles, which favors ice nucleation.

Abstract. This manuscript compiles both theoretical and experimental information on contact freezing with the aim to better understand this potentially important but still not well quantified heterogeneous freezing mode. There is no complete theory that describes contact freezing and how the energy barrier has to be overcome to nucleate an ice crystal by contact freezing. Experiments on contact freezing indicate that it can initiate ice formation at the highest temperatures. A difference in the freezing temperatures between contact and immersion freezing has been found using different instrumentation and different ice nuclei. There is a lack of data on collision rates in most of the reported data, which inhibits a quantitative calculation of the freezing efficiencies. Thus, new or modified instrumentation to study this heterogeneous freezing mode in the laboratory and in the field are needed. Important questions concerning contact freezing and its potential role for ice cloud formation and climate are also summarized.

The time dependence of immersion freezing was studied for temperatures between 236 K and 243 K. Droplets with single immersed, size-selected 400 nm and 800 nm kaolinite particles were produced at 300 K, cooled down to supercooled temperatures, and the fraction of frozen droplets with increasing residence time was detected. To simulate the conditions of immersion freezing in mixed-phase clouds we used the Zurich Ice Nucleation Chamber (ZINC) and its vertical extension, the Immersion Mode Cooling chAmber (IMCA). We observed that the frozen fraction of droplets increased with increasing residence time in the chamber. This suggests that there is a time dependence of immersion freezing and supports the importance of a stochastic component in the ice nucleation process. The rate at which droplets freeze was observed to decrease towards higher temperatures and smaller particle sizes. Comparison of the laboratory data with four different ice nucleation models, three based on classical nucleation theory with different representations of the particle surface properties and one singular, suggest that the classical, stochastic approach combined with a distribution of contact angles is able to reproduce the ice nucleation observed in these experiments most accurately. Using the models to calculate the increase in frozen fraction at typical mixed-phase cloud temperatures over an extended period of time, yields an equivalent effect of −1 K temperature shift for an increase in times scale by one order of magnitude. This suggests that temperature is more important than time.