Ice Residuals Research Articles

Preparation of long-lasting environment-friendly anti-icing agent suitable for snow and ice areas and its performance research

The addition of anti-icing agents to asphalt pavements as a way to prevent snow and ice residues should consider not only the environmental aspects of anti-icing agents, but also the water stability, high temperature stability and low temperature crack resistance of asphalt mixes. In this work, environmentally and friendly slow-release anti-icing agent called MAS was produced by using silica microspheres coated with magnesium acetate, and the performance of the mixes after adding anti-icing agents was analyzed by the water stability, high temperature stability and low temperature crack resistance tests The experimental results show that when the MAS replaces 6% of 0–0.075 mm aggregate by equal volume, the strength and performance of the mixture meet the requirements and have the best slow-release effect.

A phase separation inlet for droplets, ice residuals, and interstitial aerosol particles

Abstract. A new inlet for studying the aerosol particles and hydrometeor residuals that compose mixed-phase clouds – the phaSe seParation Inlet for Droplets icE residuals and inteRstitial aerosol particles (SPIDER) – is described here. SPIDER combines a large pumped counterflow virtual impactor (L-PCVI), a flow tube evaporation chamber, and a pumped counterflow virtual impactor (PCVI) to separate droplets, ice crystals (∼3–25 µm), and interstitial aerosol particles for simultaneous sampling. Laboratory verification tests of each individual component and the composite SPIDER system were conducted. Transmission efficiency, evaporation, and ice crystals' survival were determined to show the capability of the system. The experiments show the SPIDER system can separate distinct cloud elements and interstitial aerosol particles for subsequent analysis. As a field instrument, SPIDER will help explore the properties of different cloud elements and interstitial aerosol particles in mixed-phase clouds.

Sources and nature of ice-nucleating particles in the free troposphere at Jungfraujoch in winter 2017

Abstract. Primary ice formation in mixed-phase clouds is initiated by a minute subset of the ambient aerosol population, called ice-nucleating particles (INPs). The knowledge about their atmospheric concentration, composition, and source in cloud-relevant environments is still limited. During the 2017 joint INUIT/CLACE (Ice Nuclei research UnIT/CLoud–Aerosol Characterization Experiment) field campaign, observations of INPs as well as of aerosol physical and chemical properties were performed, complemented by source region modeling. This aimed at investigating the nature and sources of INPs. The campaign took place at the High-Altitude Research Station Jungfraujoch (JFJ), a location where mixed-phase clouds frequently occur. Due to its altitude of 3580 m a.s.l., the station is usually located in the lower free troposphere, but it can also receive air masses from terrestrial and marine sources via long-range transport. INP concentrations were quasi-continuously detected with the Horizontal Ice Nucleation Chamber (HINC) under conditions representing the formation of mixed-phase clouds at −31 ∘C. The INP measurements were performed in parallel to aerosol measurements from two single-particle mass spectrometers, the Aircraft-based Laser ABlation Aerosol MAss Spectrometer (ALABAMA) and the laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF). The chemical identity of INPs is inferred by correlating the time series of ion signals measured by the mass spectrometers with the time series of INP measurements. Moreover, our results are complemented by the direct analysis of ice particle residuals (IPRs) by using an ice-selective inlet (Ice-CVI) coupled with the ALABAMA. Mineral dust particles and aged sea spray particles showed the highest correlations with the INP time series. Their role as INPs is further supported by source emission sensitivity analysis using atmospheric transport modeling, which confirmed that air masses were advected from the Sahara and marine environments during times of elevated INP concentrations and ice-active surface site densities. Indeed, the IPR analysis showed that, by number, mineral dust particles dominated the IPR composition (∼58 %), and biological and metallic particles are also found to a smaller extent (∼10 % each). Sea spray particles are also found as IPRs (17 %), and their fraction in the IPRs strongly varied according to the increased presence of small IPRs, which is likely due to an impact from secondary ice crystal formation. This study shows the capability of combining INP concentration measurements with chemical characterization of aerosol particles using single-particle mass spectrometry, source region modeling, and analysis of ice residuals in an environment directly relevant for mixed-phase cloud formation.

A biogenic secondary organic aerosol source of cirrus ice nucleating particles

Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46 °C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L–1. Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties.

Influence of the face surface shape of the piston on the limit value of compaction stress in the process of dry ice agglomeration

This paper presents the results of research on improving the efficiency of the mechanical agglomeration through describing the influence of the shape of the piston pressure face on the limit force value. The focus of this study is the geometrical parameters which are describing the shape of the piston pressure face. Where these parameters influence on the value of the limit stress in the process of mechanical agglomeration of crystallized carbon dioxide. The first part of the paper proposes a model describing the influence of the geometric parameters of the piston pressure face on the value of axial force during the subsequent compression phase of the process. The research part of the paper presents the empirical research results to verify the proposed model. The results of the work will be used to determine the influence of the described geometrical parameters of the dry ice residue on the axial force value. The derived mathematical model will be used for defining the design requirements as the starting point for the design and building of dry ice compression and granulation machines.

Activation of intact bacteria and bacterial fragments mixed with agar as cloud droplets and ice crystals in cloud chamber experiments

Abstract. Biological particles, including bacteria and bacterial fragments, have been of much interest due to the special ability of some to nucleate ice at modestly supercooled temperatures. This paper presents results from a recent study conducted on two strains of cultivated bacteria which suggest that bacterial fragments mixed with agar, and not whole bacterial cells, serve as cloud condensation nuclei (CCN). Due to the absence of whole bacteria cells in droplets, they are unable to serve as ice nucleating particles (INPs) in the immersion mode under the experimental conditions. Experiments were conducted at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber at the Karlsruhe Institute of Technology (KIT) by injecting bacteria-containing aerosol samples into the cloud chamber and inducing cloud formation by expansion over a temperature range of −5 to −12 ∘C. Cloud droplets and ice crystals were sampled through a pumped counterflow virtual impactor inlet (PCVI) and their residuals were characterized with a single particle mass spectrometer (miniSPLAT). The size distribution of the overall aerosol was bimodal, with a large particle mode composed of intact bacteria and a mode of smaller particles composed of bacterial fragments mixed with agar that were present in higher concentrations. Results from three expansions with two bacterial strains indicate that the cloud droplet residuals had virtually the same size distribution as the smaller particle size mode and had mass spectra that closely matched those of bacterial fragments mixed with agar. The characterization of ice residuals that were sampled through an ice-selecting PCVI (IS-PCVI) also shows that the same particles that activate to form cloud droplets, bacteria fragments mixed with agar, were the only particle type observed in ice residuals. These results indicate that the unavoidable presence of agar or other growth media in all laboratory studies conducted on cultivated bacteria can greatly affect the results and needs to be considered when interpreting CCN and IN activation data.

Immersion Freezing of Total Ambient Aerosols and Ice Residuals

This laboratory study evaluates an experimental set-up to study the immersion freezing properties of ice residuals (IRs) at a temperature ranging from −26 to −34 °C using two continuous-flow diffusion chamber-style ice nucleation chambers coupled with a virtual impactor and heat exchanger. Ice was nucleated on the total ambient aerosol through an immersion freezing mechanism in an ice nucleation chamber (chamber 1). The larger ice crystals formed in chamber 1 were separated and sublimated to obtain IRs, and the frozen fraction of these IRs was investigated in a second ice nucleation chamber (chamber 2). The ambient aerosol was sampled from a sampling site located in the Columbia Plateau region, WA, USA, which is subjected to frequent windblown dust events, and only particles less than 1.5 μm in diameter were investigated. Single-particle elemental composition analyses of the total ambient aerosols showed that the majority of the particles are dust particles coated with organic matter. This study demonstrated a capability to investigate the ice nucleation properties of IRs to better understand the nature of Ice Nucleating Particles (INPs) in the ambient atmosphere.

The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review

Predicting the formation of ice in the atmosphere presents one of the great challenges in physical sciences with important implications for the chemistry and composition of the Earth’s atmosphere, the hydrological cycle, and climate. Among atmospheric ice formation processes, heterogeneous ice nucleation proceeds on aerosol particles ranging from a few nanometers to micrometers in size, commonly referred to as ice nucleating particles (INPs). Research over the last two decades has demonstrated that organic matter (OM) is ubiquitous in the atmosphere, present as organic aerosol (OA) particles or as coatings on other particle types. The physicochemical properties of OM make predicting how OM can contribute to the INP population challenging. This review focuses on the role of OM in INPs, summarizing and highlighting recent advances in our understanding of the ice nucleation process gained from theoretical, laboratory, and field studies. Examination of ice residuals and INPs with analytical techniques demonst...

Aerosol Scavenging during the Early Growth Stage of Ice Crystal Formation

This paper investigated the possibility that aerosol particles are scavenged during the first and fast diffusional growth of small ice crystals. After ice phase formation, riming, scavenging and aggregation may lead to the collection of additional aerosol particles. Therefore, particles left after ice evaporation in hydrometeors, called ice residuals, may not currently be identical to ice nucleating particles. To overcome this problem, the largest ice crystals are removed during sampling in clouds and only crystals in the initial phase of growth, with diameters lower than 20 - 30 μm, are usually considered. Published papers assume that no aerosol scavenging takes place during the initial phase of growth of small ice crystals. The aim of this paper was to ascertain if this assumption is valid. Experiments were performed in a cold laboratory by considering ice crystals growing in the presence of supercooled droplets. Results showed that crystals can scavenge aerosol even in the first stage of growth. Theoretical considerations show that aerosol scavenging cannot be explained by Brownian diffusion, inertial impaction or interception processes. We suggest that the presence of aerosol in the pristine ice crystals may be due to diffusiophoretic force. During diffusive crystal growth, a flow called Stefan’s flow exists near the hydrometeor surface, driving the nearby aerosol particles towards the surface of the growing hydrometeors.

Measurements of Ice Nucleating Particles and Ice Residuals

Abstract It has been known that aerosol particles act as nuclei for ice formation for over a century and a half (see Dufour). Initial attempts to understand the nature of these ice nucleating particles were optical and electron microscope inspection of inclusions at the center of a crystal (see Isono; Kumai). Only within the last few decades has instrumentation to extract ice crystals from clouds and analyze the residual material after sublimation of condensed-phase water been available (see Cziczo and Froyd). Techniques to ascertain the ice nucleating potential of atmospheric aerosols have only been in place for a similar amount of time (see DeMott et al.). In this chapter the history of measurements of ice nucleating particles, both in the field and complementary studies in the laboratory, are reviewed. Remaining uncertainties and artifacts associated with measurements are described and suggestions for future areas of improvement are made.

Influence of the Compression Length on the Ultimate Stress in the Process of Mechanical Agglomeration of Dry Ice

This paper presents the results of research on improving the efficiency of the mechanical agglomeration through optimising the distance to which the ram approaches the die face in the final position. The focus of this study is the influence of the compression length on the value of the ultimate stress in the process of mechanical agglomeration of crystallized carbon dioxide. The first part of the paper proposes a model describing the influence of the geometric parameters of the residual amount of material which must remain in the cylinder on the value of axial force during subsequent compression phase of the process. The research part of the paper presents the empirical research results to verify the proposed model. The results of the work will be used to determine the influence of the described geometrical parameters of the dry ice residue on the axial force value. The derived mathematical model will be used for defining the design requirements as the starting point for the design and building of dry ice compression and granulation machines.

Potential Sites for Ice Nucleation on Aluminosilicate Clay Minerals and Related Materials.

Few aerosol particles in clouds nucleate the formation of ice. The surface sites available for nucleus formation, which can include surface defects and functional groups, determine in part the activity of an aerosol particle toward ice formation. Although ice nucleation on particles has been widely studied, exploration of the specific sites at which the initial germ forms has been limited, but is important for predicting the microphysical properties of clouds, which impact climate. This Perspective focuses on what is currently known about surface sites for ice nucleation on aluminosilicate clay minerals, which are commonly found in ice residuals, as well as related materials.

The Ice Selective Inlet: a novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds

Abstract. Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol–cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of much more numerous liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterization. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artefacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the optical particle size spectrometers and a characterization of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterization Experiment (CLACE) 2013 and 2014 – two extensive international field campaigns encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaigns provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterization of its components, as well as field measurements demonstrating the ISI performance and validating the working principle of the inlet. Finally, measurements of biological aerosol during a Saharan dust event (SDE) are presented, showing a first indication of enrichment of bio-material in sub-2 μm ice residuals.

Ice nucleation by combustion ash particles at conditions relevant to mixed-phase clouds

Abstract. Ice-nucleating particles can modify cloud properties with implications for climate and the hydrological cycle; hence, it is important to understand which aerosol particle types nucleate ice and how efficiently they do so. It has been shown that aerosol particles such as natural dusts, volcanic ash, bacteria and pollen can act as ice-nucleating particles, but the ice-nucleating ability of combustion ashes has not been studied. Combustion ashes are major by-products released during the combustion of solid fuels and a significant amount of these ashes are emitted into the atmosphere either during combustion or via aerosolization of bottom ashes. Here, we show that combustion ashes (coal fly ash, wood bottom ash, domestic bottom ash, and coal bottom ash) nucleate ice in the immersion mode at conditions relevant to mixed-phase clouds. Hence, combustion ashes could play an important role in primary ice formation in mixed-phase clouds, especially in clouds that are formed near the emission source of these aerosol particles. In order to quantitatively assess the impact of combustion ashes on mixed-phase clouds, we propose that the atmospheric abundance of combustion ashes should be quantified since up to now they have mostly been classified together with mineral dust particles. Also, in reporting ice residue compositions, a distinction should be made between natural mineral dusts and combustion ashes in order to quantify the contribution of combustion ashes to atmospheric ice nucleation.

Degradation of buried ice and permafrost in the Veleta cirque (Sierra Nevada, Spain) from 2006 to 2013 as a response to recent climate trends

Abstract. The Veleta cirque is located at the foot of the Veleta peak, one of the highest summits of the Sierra Nevada National Park (southern Spain). This cirque was the source of a glacier valley during the Quaternary cold periods. During the Little Ice Age it sheltered a small glacier, the most southerly in Europe, about which we have possessed written records since the 17th century. This glacier still had ice residues until the mid-20th century. This ice is no longer visible, but a residue persists along with discontinuous permafrost trapped under strata of rock blocks that make up an incipient rock glacier. From 2006 to 2013, this rock glacier was monitored by measurement of the temperature of the active layer, the degree of snow cover on the ground, movements of the body of the rock glacier and geophysical prospection inside it. The results show that the relict ice and trapped permafrost have been steadily declining. The processes that explain this degradation occur in chain, starting from the external radiation that affects the ground in summer, which is when the temperatures are higher. In effect, when this radiation steadily melts the snow on the ground, the thermal expansive wave advances into the heart of the active layer, reaching the ceiling of the frozen mass, which it then degrades and melts. In this entire linked process, the circulation of meltwaters fulfils a highly significant function, as they act as heat transmitters. The complementary nature of these processes explains the subsidence and continuous changes in the entire clastic pack and the melting of the frozen ceiling on which it rests. This happens in summer in just a few weeks. All these events, in particular the geomorphological ones, take place on the Sierra Nevada peaks within certain climate conditions that are at present unfavourable to the maintenance of snow on the ground in summer. These conditions could be related to recent variations in the climate, starting in the mid-19th century and most markedly since the second half of the 20th century. The work and results highlight the climate sensitivity of the peaks of the Sierra Nevada to the effect of climate change and its impact on the dynamics of ecosystems, which is a benchmark for evaluating the current evolution of landscapes of Mediterranean high mountains.

Heterogeneous Ice Nucleation on Simulated Sea-Spray Aerosol Using Raman Microscopy

The deliquescence and heterogeneous ice nucleation behavior of simulated sea-spray aerosol was probed from 215 to 235 K using Raman microscopy coupled to an environmental cell. Water uptake prior to deliquescence was also probed on sea-salt particles along deliquescence/ice nucleation experimental trajectories. Synthetic sea-salt particles were generated from solutions of aquarium salt, which emulates all major and minor ions that are found in saltwater. Our results indicate that, under cirrus cloud conditions, sea-salt particles will be in an internally mixed liquid–solid phase, with a brine layer surrounding a crystalline core. Above 230 K, the core of the internally mixed liquid–solid particle fully deliquesces prior to ice nucleation. Below 225 K, however, the crystalline core can act as an efficient immersion-mode ice nuclei prior to full liquefaction. To simulate the presence of carbohydrate-like organics in sea-spray aerosol, sea-salt particles were mixed with the disaccharide sucrose 1:1 by mass. At low relative humidity, the sea-salt particles effloresced into an amorphous organic-salt matrix. Above 225 K, sea-salt/sucrose particles fully deliquesce prior to ice nucleation; however, at lower temperatures, the organic-salt matrix was found to be glassy and could act as an efficient heterogeneous ice nucleus. This work suggests the possible role of sea-salt aerosol in low-temperature ice nucleation. Consistent with this, data from aircraft campaigns suggests sea-salt aerosol is enhanced in ice residuals from low-temperature anvil cirrus whose convective inflow regions are primarily marine environments.

Investigation of pyridine carboxylic acids in CM2 carbonaceous chondrites: Potential precursor molecules for ancient coenzymes

The distribution and abundances of pyridine carboxylic acids (including nicotinic acid) in eight CM2 carbonaceous chondrites (ALH 85013, DOM 03183, DOM 08003, EET 96016, LAP 02333, LAP 02336, LEW 85311, and WIS 91600) were investigated by liquid chromatography coupled to UV detection and high resolution Orbitrap mass spectrometry. We find that pyridine monocarboxylic acids are prevalent in CM2-type chondrites and their abundance negatively correlates with the degree of pre-terrestrial aqueous alteration that the meteorite parent body experienced. We also report the first detection of pyridine dicarboxylic acids in carbonaceous chondrites. Additionally, we carried out laboratory studies of proton-irradiated pyridine in carbon dioxide-rich ices (a 1:1 mixture) to serve as a model of the interstellar ice chemistry that may have led to the synthesis of pyridine carboxylic acids. Analysis of the irradiated ice residue shows that a comparable suite of pyridine mono- and dicarboxylic acids was produced, although aqueous alteration may still play a role in the synthesis (and ultimate yield) of these compounds in carbonaceous meteorites. Nicotinic acid is a precursor to nicotinamide adenine dinucleotide, a likely ancient molecule used in cellular metabolism in all of life, and its common occurrence in CM2 chondrites may indicate that meteorites may have been a source of molecules for the emergence of more complex coenzymes on the early Earth.

Studies of propane flame soot acting as heterogeneous ice nuclei in conjunction with single particle soot photometer measurements

Abstract. The ice nucleation efficiency of propane flame soot particles with and without a sulphuric acid coating was investigated using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere). The test soot for cloud formation simulations was produced using a propane flame Combustion Aerosol Standard generator (CAST, Jing-CAST Technologies). The organic carbon content (OC) of the test soot was altered in a reproducible fashion by changing the fuel/air mixture of the generator. The soot content of ice nuclei was subsequently investigated using a combination of a pumped counterflow virtual impactor (PCVI) to separate and evaporate the ice crystals, and a DMT single particle soot photometer (SP2) to examine the mixing state of the BC containing ice residuals. Ice nucleation was found to be most efficient for uncoated soot of low organic carbon content (~5 % organic carbon content) where deposition freezing occurred at an ice saturation ratio Sice ~ 1.22 at a temperature T = 226.6 K with 25 % of the test soot becoming active as ice nuclei. Propane flame soot of higher organic carbon content (~30 % and ~70 % organic carbon content) showed significantly lower ice nucleation efficiency (an activated fraction of the order of a few percent in the experiments) than the low organic carbon content soot, with water saturation being required for freezing to occur. Ice nucleation occurred over the range Sice = 1.22–1.70, and T = 223.2–226.6 K. Analysis of the SP2 data showed that the 5 % organic carbon content soot had an undetectable OC coating whereas the 30 % organic carbon content soot had a thicker or less volatile OC coating. The application of a sulphuric acid coating to the flame soot shifted the threshold of the onset of freezing towards that of the homogeneous freezing of sulphuric acid; for the minimum OC flame soot this inhibited nucleation since the onset of freezing occurred at colder temperatures and required a greater ice saturation ratio; for the medium and maximum OC flame soot, the addition of a sulphuric acid significantly reduced the freezing threshold.

Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds

Abstract. During an intensive campaign at the high alpine research station Jungfraujoch, Switzerland, in February/March 2006 ice particle residuals within mixed-phase clouds were sampled using the Ice-counterflow virtual impactor (Ice-CVI). Size, morphology, chemical composition, mineralogy and mixing state of the ice residual and the interstitial (i.e., non-activated) aerosol particles were analyzed by scanning and transmission electron microscopy. Ice nuclei (IN) were identified from the significant enrichment of particle groups in the ice residual (IR) samples relative to the interstitial aerosol. In terms of number lead-bearing particles are enriched by a factor of approximately 25, complex internal mixtures with silicates or metal oxides as major components by a factor of 11, and mixtures of secondary aerosol and carbonaceous material (C-O-S particles) by a factor of 2. Other particle groups (sulfates, sea salt, Ca-rich particles, external silicates) observed in the ice-residual samples cannot be assigned unambiguously as IN. Between 9 and 24% of all IR are Pb-bearing particles. Pb was found as major component in around 10% of these particles (PbO, PbCl2). In the other particles, Pb was found as some 100 nm sized agglomerates consisting of 3–8 nm sized primary particles (PbS, elemental Pb). C-O-S particles are present in the IR at an abundance of 17–27%. The soot component within these particles is strongly aged. Complex internal mixtures occur in the IR at an abundance of 9–15%. Most IN identified at the Jungfraujoch station are internal mixtures containing anthropogenic components (either as main or minor constituent), and it is concluded that admixture of the anthropogenic component is responsible for the increased IN efficiency within mixed phase clouds. The mixing state appears to be a key parameter for the ice nucleation behaviour that cannot be predicted from the sole knowledge of the main component of an individual particle.

Chemical composition of ambient aerosol, ice residues and cloud droplet residues in mixed-phase clouds: single particle analysis during the Cloud and Aerosol Characterization Experiment (CLACE 6)

Abstract. Two different single particle mass spectrometers were operated in parallel at the Swiss High Alpine Research Station Jungfraujoch (JFJ, 3580 m a.s.l.) during the Cloud and Aerosol Characterization Experiment (CLACE 6) in February and March 2007. During mixed phase cloud events ice crystals from 5–20 μm were separated from larger ice aggregates, non-activated, interstitial aerosol particles and supercooled droplets using an Ice-Counterflow Virtual Impactor (Ice-CVI). During one cloud period supercooled droplets were additionally sampled and analyzed by changing the Ice-CVI setup. The small ice particles and droplets were evaporated by injection into dry air inside the Ice-CVI. The resulting ice and droplet residues (IR and DR) were analyzed for size and composition by the two single particle mass spectrometers: a custom-built Single Particle Laser-Ablation Time-of-Flight Mass Spectrometer (SPLAT) and a commercial Aerosol Time-of-Flight Mass Spectrometer (ATOFMS, TSI Model 3800). During CLACE 6 the SPLAT instrument characterized 355 individual IR that produced a mass spectrum for at least one polarity and the ATOFMS measured 152 IR. The mass spectra were binned in classes, based on the combination of dominating substances, such as mineral dust, sulfate, potassium and elemental carbon or organic material. The derived chemical information from the ice residues is compared to the JFJ ambient aerosol that was sampled while the measurement station was out of clouds (several thousand particles analyzed by SPLAT and ATOFMS) and to the composition of the residues of supercooled cloud droplets (SPLAT: 162 cloud droplet residues analyzed, ATOFMS: 1094). The measurements showed that mineral dust was strongly enhanced in the ice particle residues. Close to all of the SPLAT spectra from ice residues did contain signatures from mineral compounds, albeit connected with varying amounts of soluble compounds. Similarly, close to all of the ATOFMS IR spectra show a mineral or metallic component. Pure sulfate and nitrate containing particles were depleted in the ice residues. Sulfate and nitrate was found to dominate the droplet residues (~90% of the particles). The results from the two different single particle mass spectrometers were generally in agreement. Differences in the results originate from several causes, such as the different wavelength of the desorption and ionisation lasers and different size-dependent particle detection efficiencies.