Ice crystal numbers can exceed the numbers of icenucleating particles (INPs) observed in mixed-phase clouds (MPCs) by several orders of magnitude, also at temperatures that are colder than − 8 • C. This disparity provides circumstantial evidence of secondary ice formation, also other than via the Hallett-Mossop process. In a new approach, we made use of the fact that planar, branched ice crystals (e.g. dendrites) grow within a relatively narrow temperature range (i.e. −12 to −17 • C) and can be analysed individually for INPs using a field-deployable drop-freezing assay. The novelty of our approach lies in comparing the growth temperature encoded in the habit of an individual crystal with the activation temperature of the most efficient INP contained within the same crystal to tell whether it may be the result of primary ice formation. In February and March 2018, we analysed a total of 190 dendritic crystals (∼ 3 mm median size) deposited within MPCs at the high-altitude research station Jungfraujoch (3580 m a.s.l.). Overall, one in eight of the analysed crystals contained an INP active at −17 • C or warmer, while the remaining seven most likely resulted from secondary ice formation within the clouds. The ice multiplication factor we observed was small (8), but relatively stable throughout the course of documentation. These measurements show that secondary ice can be observed at temperatures around −15 • C and thus advance our understanding of the extent of secondary ice formation in MPCs, even where the multiplication factor is smaller than 10.

Abstract. An accurate prediction of the ice crystal number concentration in clouds is important to determine the radiation budget, the lifetime, and the precipitation formation of clouds. Secondary-ice production is thought to be responsible for the observed discrepancies between the ice crystal number concentration and the ice-nucleating particle concentration in clouds. The Hallett–Mossop process is active between −3 and −8 ∘C and has been implemented into several models, while all other secondary-ice processes are poorly constrained and lack a well-founded quantification. During 2 h of measurements taken on a mountain slope just above the melting layer at temperatures warmer than −3 ∘C, a continuously high concentration of small plates identified as secondary ice was observed. The presence of drizzle drops suggests droplet fragmentation upon freezing as the responsible secondary-ice mechanism. The constant supply of drizzle drops can be explained by a recirculation theory, suggesting that melted snowflakes, which sedimented through the melting layer, were reintroduced into the cloud as drizzle drops by orographically forced updrafts. Here we introduce a parametrization of droplet fragmentation at slightly sub-zero temperatures, where primary-ice nucleation is basically absent, and the first ice is initiated by the collision of drizzle drops with aged ice crystals sedimenting from higher altitudes. Based on previous measurements, we estimate that a droplet of 200 µm in diameter produces 18 secondary-ice crystals when it fragments upon freezing. The application of the parametrization to our measurements suggests that the actual number of splinters produced by a fragmenting droplet may be up to an order of magnitude higher.

Abstract. The seeder–feeder mechanism has been observed to enhance orographic precipitation in previous studies. However, the microphysical processes active in the seeder and feeder region are still being understood. In this paper, we investigate the seeder and feeder region of a mixed-phase cloud passing over the Swiss Alps, focusing on (1) fallstreaks of enhanced radar reflectivity originating from cloud top generating cells (seeder region) and (2) a persistent low-level feeder cloud produced by the boundary layer circulation (feeder region). Observations were obtained from a multi-dimensional set of instruments including ground-based remote sensing instrumentation (Ka-band polarimetric cloud radar, microwave radiometer, wind profiler), in situ instrumentation on a tethered balloon system, and ground-based aerosol and precipitation measurements. The cloud radar observations suggest that ice formation and growth were enhanced within cloud top generating cells, which is consistent with previous observational studies. However, uncertainties exist regarding the dominant ice formation mechanism within these cells. Here we propose different mechanisms that potentially enhance ice nucleation and growth in cloud top generating cells (convective overshooting, radiative cooling, droplet shattering) and attempt to estimate their potential contribution from an ice nucleating particle perspective. Once ice formation and growth within the seeder region exceeded a threshold value, the mixed-phase cloud became fully glaciated. Local flow effects on the lee side of the mountain barrier induced the formation of a persistent low-level feeder cloud over a small-scale topographic feature in the inner-Alpine valley. In situ measurements within the low-level feeder cloud observed the production of secondary ice particles likely due to the Hallett–Mossop process and ice particle fragmentation upon ice–ice collisions. Therefore, secondary ice production may have been partly responsible for the elevated ice crystal number concentrations that have been previously observed in feeder clouds at mountaintop observatories. Secondary ice production in feeder clouds can potentially enhance orographic precipitation.

Abstract. A small fraction of freezing cloud droplets probably initiates much of the precipitation above continents. Only a minute fraction of aerosol particles, so-called ice-nucleating particles (INPs), can trigger initial ice formation at −15 ∘C, at which cloud-top temperatures are frequently associated with snowfall. At a mountaintop site in the Swiss Alps, we found that concentrations of INPs active at −15 ∘C can be parameterised by different functions of coarse (> 2 µm) aerosol particle concentrations, depending on whether an air mass is (a) precipitating, (b) non-precipitating, or (c) carrying a substantial fraction of dust particles while non-precipitating. Consequently, we suggest that a parameterisation at moderate supercooling should consider coarse particles in combination with air mass differentiation.

Abstract. Aerosol–cloud interactions, including the ice nucleation of supercooled liquid water droplets caused by ice-nucleating particles (INPs) and macromolecules (INMs), are a source of uncertainty in predicting future climate. Because INPs and INMs have spatial and temporal heterogeneity in source, number, and composition, predicting their concentration and distribution is a challenge requiring apt analytical instrumentation. Here, we present the development of our drop Freezing Ice Nuclei Counter (FINC) for the estimation of INP and INM concentrations in the immersion freezing mode. FINC's design builds upon previous droplet freezing techniques (DFTs) and uses an ethanol bath to cool sample aliquots while detecting freezing using a camera. Specifically, FINC uses 288 sample wells of 5–60 µL volume, has a limit of detection of −25.4 ± 0.2 ∘C with 5 µL, and has an instrument temperature uncertainty of ± 0.5 ∘C. We further conducted freezing control experiments to quantify the nonhomogeneous behavior of our developed DFT, including the consideration of eight different sources of contamination. As part of the validation of FINC, an intercomparison campaign was conducted using an NX-illite suspension and an ambient aerosol sample from two other drop freezing instruments: ETH's DRoplet Ice Nuclei Counter Zurich (DRINCZ) and the University of Basel's LED-based Ice Nucleation Detection Apparatus (LINDA). We also tabulated an exhaustive list of peer-reviewed DFTs, to which we added our characterized and validated FINC. In addition, we propose herein the use of a water-soluble biopolymer, lignin, as a suitable ice-nucleating standard. An ideal INM standard should be inexpensive, accessible, reproducible, unaffected by sample preparation, and consistent across techniques. First, we compared lignin's freezing temperature across different drop freezing instruments, including on DRINCZ and LINDA, and then determined an empirical fit parameter for future drop freezing validations. Subsequently, we showed that commercial lignin has consistent ice-nucleating activity across product batches and demonstrated that the ice-nucleating ability of aqueous lignin solutions is stable over time. With these findings, we present lignin as a good immersion freezing standard for future DFT intercomparisons in the research field of atmospheric ice nucleation.