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Volcanic ash (VA) from explosive eruptions contributes to aerosol loadings in the atmosphere. Aside from the negative impact of VA on air quality and aviation, these particles can alter the optical and microphysical properties of clouds by triggering ice formation, thereby influencing precipitation and climate. Depending on the volcano and eruption style, VA displays a wide range of different physical, chemical, and mineralogical properties. Here, we present a unique data set on the ice nucleation activity of 15 VA samples obtained from different volcanoes worldwide. The ice nucleation activities of these samples were studied in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud simulation chamber as well as with the Ice Nucleation Spectrometer of the Karlsruhe Institute of Technology (INSEKT). All VA particles nucleated ice in the immersion freezing mode from 263 to 238K with ice nucleation active site (INAS) densities ranging from ∼105 to 1011 m−2, respectively. The variabilities observed among the VA samples, at any given temperature, range over 3.5 orders of magnitude. The ice‐nucleating abilities of VA samples correlate to varying degrees with their bulk pyroxene and plagioclase contents as a function of temperature. We combined our new data set with existing literature data to develop an improved ice nucleation parameterization for natural VA in the immersion freezing mode. This should be useful for modeling the impact of VA on clouds., Plain Language Summary: Volcanic ash particles, which are generated during volcanic eruptions, can initiate ice formation in clouds. The clouds formed by these volcanic ash particles can influence precipitation, and in turn, weather and climate. In our study, we investigated the ability with which volcanic ash particles form ice in clouds. We performed our study in a state‐of‐the‐art aerosol and cloud simulation chamber and on a cold‐stage instrument. The findings show that volcanic ash particles can form ice as effectively as mineral dust particles or their components. These results will help scientists to have a better understanding of the impact of volcanic ash particles on clouds., Key Points: The ice‐nucleating ability of natural volcanic ash particles in the immersion freezing mode can vary by 3.5 orders of magnitude. Ice‐nucleating properties of volcanic ash particles correlate to varying degrees with their pyroxene and plagioclase contents. The temperature‐dependent immersion freezing ability of volcanic ash is approximated with an exponential fit line., Alexander von Humboldt‐Stiftung (Humboldt‐Stiftung) http://dx.doi.org/10.13039/100005156, Marie Skłodowska‐Curie Actions, ERC 2018 ADG, Deutsche Forschungsgemeinschaft (DFG) http://dx.doi.org/10.13039/501100001659, Helmholtz Association of German Research Centres, EUROCHAMP 2020 Infrastructure Activity

This study presents a comprehensive investigation of ice-nucleating particles (INPs) in the surface materials and aerosol particles from U.S. cattle feeding facilities. Using a modern suite of online and offline aerosol particle characterization instruments, we conducted a three-year field survey (2016–2019), Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber experiments, and ice crystal residual (ICR) analyses for the feedlot sample. Our results showed unique supermicron size dominance in the feedlot INPs with a high concentration of INPs (several hundred and thousand INPs L−1 at −20 °C and −25 °C, respectively). Thus, agricultural fields, especially animal feeding facilities, represent important INP sources if these particles rise to sufficient height in the atmosphere. New data on the ice nucleation (IN) properties of agricultural dust at heterogeneous freezing temperatures (Ts > −29 °C) were generated, providing statistical context. Overall, we successfully characterized physical, chemical, and biological properties of aerosol particles found at a cattle feedlot, thereby finding their unique heat-tolerant nature. The relationship between these measured properties and atmospheric IN parameterization relevant to mixed-phase clouds is discussed. Our INP parameterization and ICR characterization are meaningful for improved understanding of INP emission and cloud microphysical processes in the supermicron-particle laden region. These unique INPs may directly influence the lifetime of supercooled clouds in a unique manner for this region. An application of our IN parameterization is crucial to explore INP relations to supercooled cloud properties over such a predominant agricultural area.

In spite of the resurgence in ice nucleation research a comparatively small number of studies deal with the phenomenon of pre-activation in heterogeneous ice nucleation. Fifty years ago, it was shown that various mineral dust and volcanic ash particles can be pre-activated to become nuclei for ice crystal formation even at temperatures as high as 270–271 K. Pre-activation was achieved under ice-subsaturated conditions without any preceding macroscopic ice growth by just temporarily cooling the particles to temperatures below 228 K. A two-step mechanism involving capillary condensation of supercooled water and subsequent homogeneous freezing was proposed to account for the particles' enhanced ice nucleation ability at high temperatures. This work reinvestigates the efficiency of the proposed pre-activation mechanism in temperature-cycling experiments performed in a large cloud chamber with suspended particles. We find the efficiency to be highest for the clay mineral illite as well as for highly porous materials like zeolite and diatomaceous earth, whereas most aerosols generated from desert dust surface samples did not reveal a measurable pre-activation ability. The pre-activation efficiency is linked to particle pores in a certain size range. As estimated by model calculations, only pores with diameters between about 5 and 8 nm contribute to pre-activation under ice-subsaturated conditions. This range is set by a combination of requirements from the negative Kelvin effect for condensation and a critical size of ice embryos for ice nucleation and melting. In contrast to the early study, pre-activation is only observed for temperatures below 260 K. Above that threshold, the particles' improved ice nucleation ability disappears due to the melting of ice in the pores.

Seven different instruments and measurement methods were used to examine the immersion freezing of bacterial ice nuclei from Snomax® (hereafter Snomax), a product containing ice-active protein complexes from non-viable Pseudomonas syringae bacteria. The experimental conditions were kept as similar as possible for the different measurements. Of the participating instruments, some examined droplets which had been made from suspensions directly, and the others examined droplets activated on previously generated Snomax particles, with particle diameters of mostly a few hundred nanometers and up to a few micrometers in some cases. Data were obtained in the temperature range from −2 to −38 °C, and it was found that all ice-active protein complexes were already activated above −12 °C. Droplets with different Snomax mass concentrations covering 10 orders of magnitude were examined. Some instruments had very short ice nucleation times down to below 1 s, while others had comparably slow cooling rates around 1 K min−1. Displaying data from the different instruments in terms of numbers of ice-active protein complexes per dry mass of Snomax, nm, showed that within their uncertainty, the data agree well with each other as well as to previously reported literature results. Two parameterizations were taken from literature for a direct comparison to our results, and these were a time-dependent approach based on a contact angle distribution (Niedermeier et al., 2014) and a modification of the parameterization presented in Hartmann et al. (2013) representing a time-independent approach. The agreement between these and the measured data were good; i.e., they agreed within a temperature range of 0.6 K or equivalently a range in nm of a factor of 2. From the results presented herein, we propose that Snomax, at least when carefully shared and prepared, is a suitable material to test and compare different instruments for their accuracy of measuring immersion freezing.

During the eruption of the Eyjafjallajökull volcano in the south of Iceland in April/May 2010, about 40 Tg of ash mass were emitted into the atmosphere. It was unclear whether volcanic ash particles with d < 10 μm facilitate the glaciation of clouds. Thus, ice nucleation properties of volcanic ash particles were investigated in AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber experiments simulating atmospherically relevant conditions. The ash sample that was used for our experiments had been collected at a distance of 58 km from the Eyjafjallajökull during the eruption period in April 2010. The temperature range covered by our ice nucleation experiments extended from 219 to 264 K, and both ice nucleation via immersion freezing and deposition nucleation could be observed. Immersion freezing was first observed at 252 K, whereas the deposition nucleation onset lay at 242 K and RHice =126%. About 0.1% of the volcanic ash particles were active as immersion freezing nuclei at a temperature of 249 K. For deposition nucleation, an ice fraction of 0.1% was observed at around 233 K and RHice =116%. Taking ice-active surface site densities as a measure for the ice nucleation efficiency, volcanic ash particles are similarly efficient ice nuclei in immersion freezing mode (ns,imm ~ 109 m−2 at 247 K) compared to certain mineral dusts. For deposition nucleation, the observed ice-active surface site densities ns,dep were found to be 1011 m−2 at 224 K and RHice =116%. Thus, volcanic ash particles initiate deposition nucleation more efficiently than Asian and Saharan dust but appear to be poorer ice nuclei than ATD particles. Based on the experimental data, we have derived ice-active surface site densities as a function of temperature for immersion freezing and of relative humidity over ice and temperature for deposition nucleation.

Deposition nucleation experiments with Arizona Test Dust (ATD) as a surrogate for mineral dusts were conducted at the AIDA cloud chamber at temperatures between 220 and 250 K. The influence of the aerosol size distribution and the cooling rate on the ice nucleation efficiencies was investigated. Ice nucleation active surface site (INAS) densities were calculated to quantify the ice nucleation efficiency as a function of temperature, humidity and the aerosol surface area concentration. Additionally, a contact angle parameterization according to classical nucleation theory was fitted to the experimental data in order to relate the ice nucleation efficiencies to contact angle distributions. From this study it can be concluded that the INAS density formulation is a very useful tool to describe the temperature- and humidity-dependent ice nucleation efficiency of ATD particles. Deposition nucleation on ATD particles can be described by a temperature- and relative-humidity-dependent INAS density function ns(T, Sice) with ns(xtherm) = 1.88 ×105 · exp(0.2659 · xtherm) [m−2] , (1) where the temperature- and saturation-dependent function xtherm is defined as xtherm = −(T−273.2)+(Sice−1) ×100, (2) with the saturation ratio with respect to ice Sice >1 and within a temperature range between 226 and 250 K. For lower temperatures, xtherm deviates from a linear behavior with temperature and relative humidity over ice. Also, two different approaches for describing the time dependence of deposition nucleation initiated by ATD particles are proposed. Box model estimates suggest that the time-dependent contribution is only relevant for small cooling rates and low number fractions of ice-active particles.

Soil dust particles emitted from agricultural areas contain considerable mass fractions of organic material. Also, soil dust particles may act as carriers for potentially ice-active biological particles. In this work, we present ice nucleation experiments conducted in the AIDA cloud chamber. We investigated the ice nucleation efficiency of four types of soil dust from different regions of the world. The results are expressed as ice nucleation active surface site (INAS) densities and presented for the immersion freezing and the deposition nucleation mode. For immersion freezing occurring at 254 K, samples from Argentina, China and Germany show ice nucleation efficiencies which are by a factor 10 higher than desert dusts. On average, the difference in ice nucleation efficiencies between agricultural and desert dusts becomes significantly smaller at temperatures below 247 K. In the deposition mode the soil dusts showed higher ice nucleation activity than Arizona Test Dust over a temperature range between 232 and 248 K, and humidities RHice up to 125%. INAS densities varied between 109 and 1011 m-2 for these thermodynamic conditions. For one soil dust sample (Argentinian Soil), the effect of treatments with heat was investigated. Heat treatments (383 K) did not affect the ice nucleation efficiency observed at 249 K. This finding presumably excludes proteinaceous ice nucleating entities as the only source of the increased ice nucleation efficiency.

A new heterogeneous ice nucleation parameterization that covers a wide temperature range (−36 to −78 °C) is presented. Developing and testing such an ice nucleation parameterization, which is constrained through identical experimental conditions, is important to accurately simulate the ice nucleation processes in cirrus clouds. The ice nucleation active surface-site density (ns) of hematite particles, used as a proxy for atmospheric dust particles, were derived from AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber measurements under water subsaturated conditions. These conditions were achieved by continuously changing the temperature (T) and relative humidity with respect to ice (RHice) in the chamber. Our measurements showed several different pathways to nucleate ice depending on T and RHice conditions. For instance, almost T-independent freezing was observed at −60 °C < T < −50 °C, where RHice explicitly controlled ice nucleation efficiency, while both T and RHice played roles in other two T regimes: −78 °C < T < −60 °C and −50 °C < T < −36 °C. More specifically, observations at T lower than −60 °C revealed that higher RHice was necessary to maintain a constant ns, whereas T may have played a significant role in ice nucleation at T higher than −50 °C. We implemented the new hematite-derived ns parameterization, which agrees well with previous AIDA measurements of desert dust, into two conceptual cloud models to investigate their sensitivity to the new parameterization in comparison to existing ice nucleation schemes for simulating cirrus cloud properties. Our results show that the new AIDA-based parameterization leads to an order of magnitude higher ice crystal concentrations and to an inhibition of homogeneous nucleation in lower-temperature regions. Our cloud simulation results suggest that atmospheric dust particles that form ice nuclei at lower temperatures, below −36 °C, can potentially have a stronger influence on cloud properties, such as cloud longevity and initiation, compared to previous parameterizations.

Based on laboratory studies it has been suggested that the most important atmospheric aerosol particles acting as ice nuclei for heterogeneous freezing of cloud droplets at temperatures above −15°C could be from biological sources. Here we present simulations with a regional atmospheric model to investigate their impact on mixed-phase clouds based on recent experimental studies with different biological ice nuclei.

Since 2003, the AIDA cloud chamber has been used for comprehensive series of ice nucleation experiments with a variety of different aerosols and in wide ranges of temperature, relative humidity and cooling rate. Ice nucleation onset and ice formation rates have been obtained as a function of aerosol parameters, ice supersaturation, temperature and cooling rate for homogeneous freezing of water droplets and solution particles, immersion freezing at and below water saturation, and deposition ice nucleation between ice and water saturation. The AIDA team has started a consistent and comprehensive re-analysis of the 10 year data set to provide a new set of parameters for formulating the ice formation in atmospheric models as function of aerosol properties, temperature and humidity. Here we present basic concepts and some selected results.