Airborne investigation of black carbon interaction with low-level, persistent, mixed-phase clouds in the Arctic summer

Aerosol–cloud interaction is considered one of the largest sources of uncertainty in radiative forcing estimations. To better understand the role of black carbon (BC) aerosol as a cloud nucleus and the impact of clouds on its vertical distribution in the Arctic, we report airborne in situ measurements of BC particles in the European Arctic near Svalbard during the “Arctic CLoud Observations Using airborne measurements during polar Day” (ACLOUD) campaign held in the summer of 2017. BC was measured with a single-particle soot photometer aboard the Polar 6 research aircraft from the lowest atmospheric layer up to approximately 3500 m a.s.l (metres above sea level). During in-cloud flight transects, BC particles contained in liquid droplets (BC residuals) were sampled through a counterflow virtual impactor (CVI) inlet. Four flights, conducted in the presence of low-level, surface-coupled, inside-inversion, and mixed-phase clouds over sea ice, were selected to address the variability in BC above, below, and within the cloud layer. First, the increase in size and coating thickness of BC particles from the free troposphere to the cloud-dominated boundary layer confirmed that ground observations were not representative of upper atmospheric layers. Second, although only 1 % of liquid droplets contained a BC particle, the higher number concentration of BC residuals than BC particles sampled below cloud indicated that the totality of below-cloud BC was activated by nucleation scavenging but also that alternative scavenging processes such as the activation of free-tropospheric BC at the cloud top might occur. Third, the efficient exchange of aerosol particles at cloud bottom was confirmed by the similarity of the size distribution of BC residuals and BC particles sampled below cloud. Last, the increase in the BC residual number concentration (+31 %) and geometric mean diameter (+38 %) from the cloud top to the cloud bottom and the absolute enrichment in larger BC residuals compared with outside of the cloud supported the hypothesis of concomitant scavenging mechanisms but also suggested the formation of BC agglomerates caused by cloud processing. The vertical evolution of BC properties from inside the cloud and below the cloud indicated an efficient aerosol exchange at cloud bottom, which might include activation, cloud processing, and sub-cloud release of processed BC agglomerates. In the case of persistent low-level Arctic clouds, this cycle may reiterate multiple times, adding an additional degree of complexity to the understanding of cloud processing of BC particles in the Arctic.</p

A comprehensive characterization of ice nucleation by three different types of cellulose particles immersed in water

We present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice-nucleating plant structural polymers. These samples include microcrystalline cellulose (MCC), fibrous cellulose (FC) and nanocrystalline cellulose (NCC). Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at 17 different institutions, including nine dry dispersion and 11 aqueous suspension techniques. With a total of 20 methods, we performed systematic accuracy and precision analysis of measurements from all 20 measurement techniques by evaluating T-binned (1 ∘C) data over a wide T range (−36 ∘C <T<−4 ∘C). Specifically, we intercompared the geometric surface area-based ice nucleation active surface site (INAS) density data derived from our measurements as a function of T, ns,geo(T). Additionally, we also compared the ns,geo(T) values and the freezing spectral slope parameter (Δlog(ns,geo)/ΔT) from our measurements to previous literature results. Results show all three cellulose materials are reasonably ice active. The freezing efficiencies of NCC samples agree reasonably well, whereas the diversity for the other two samples spans ≈ 10 ∘C. Despite given uncertainties within each instrument technique, the overall trend of the ns,geo(T) spectrum traced by the T-binned average of measurements suggests that predominantly supermicron-sized cellulose particles (MCC and FC) generally act as more efficient ice-nucleating particles (INPs) than NCC with about 1 order of magnitude higher ns,geo(T)

Atmospheric and Surface Processes, and Feedback Mechanisms Determining Arctic Amplification: A Review of First Results and Prospects of the (AC)3 Project

Mechanisms behind the phenomenon of Arctic amplification are widely discussed. To contribute to this debate, the (AC)3 project has been established in 2016. It comprises modeling and data analysis efforts as well as observational elements. The project has assembled a wealth of ground-based, airborne, ship-borne, and satellite data of physical, chemical, and meteorological properties of the Arctic atmosphere, cryosphere, and upper ocean that are available for the Arctic climate research community. Short-term changes and indications of long-term trends in Arctic climate parameters have been detected using existing and new data

The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements

The second phase of the Fifth International Ice Nucleation Workshop (FIN-02) involved the gathering of a large number of researchers at the Karlsruhe Institute of Technology's Aerosol Interactions and Dynamics of the Atmosphere (AIDA) facility to promote characterization and understanding of ice nucleation measurements made by a variety of methods used worldwide. Compared to the previous workshop in 2007, participation was doubled, reflecting a vibrant research area. Experimental methods involved sampling of aerosol particles by direct processing ice nucleation measuring systems from the same volume of air in separate experiments using different ice nucleating particle (INP) types, and collections of aerosol particle samples onto filters or into liquid for sharing amongst measurement techniques that post-process these samples. In this manner, any errors introduced by differences in generation methods when samples are shared across laboratories were mitigated. Furthermore, as much as possible, aerosol particle size distribution was controlled so that the size limitations of different methods were minimized. The results presented here use data from the workshop to assess the comparability of immersion freezing measurement methods activating INPs in bulk suspensions, methods that activate INPs in condensation and/or immersion freezing modes as single particles on a substrate, continuous flow diffusion chambers (CFDCs) directly sampling and processing particles well above water saturation to maximize immersion and subsequent freezing of aerosol particles, and expansion cloud chamber simulations in which liquid cloud droplets were first activated on aerosol particles prior to freezing. The AIDA expansion chamber measurements are expected to be the closest representation to INP activation in atmospheric cloud parcels in these comparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX and potassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam (Argentina) and highly erodible sandy dryland (Tunisia) soils, respectively, and a bacterial INP (Snomax®). Considered together, the agreement among post-processed immersion freezing measurements of the numbers and fractions of particles active at different temperatures following bulk collection of particles into liquid was excellent, with possible temperature uncertainties inferred to be a key factor in determining INP uncertainties. Collection onto filters for rinsing versus directly into liquid in impingers made little difference. For methods that activated collected single particles on a substrate at a controlled humidity at or above water saturation, agreement with immersion freezing methods was good in most cases, but was biased low in a few others for reasons that have not been resolved, but could relate to water vapor competition effects. Amongst CFDC-style instruments, various factors requiring (variable) higher supersaturations to achieve equivalent immersion freezing activation dominate the uncertainty between these measurements, and for comparison with bulk immersion freezing methods. When operated above water saturation to include assessment of immersion freezing, CFDC measurements often measured at or above the upper bound of immersion freezing device measurements, but often underestimated INP concentration in comparison to an immersion freezing method that first activates all particles into liquid droplets prior to cooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber–Portable Ice Nucleation Chamber), and typically slightly underestimated INP number concentrations in comparison to cloud parcel expansions in the AIDA chamber; this can be largely mitigated when it is possible to raise the relative humidity to sufficiently high values in the CFDCs, although this is not always possible operationally. Correspondence of measurements of INPs among direct sampling and post-processing systems varied depending on the INP type. Agreement was best for Snomax® particles in the temperature regime colder than −10 ∘C, where their ice nucleation activity is nearly maximized and changes very little with temperature. At temperatures warmer than −10 ∘C, Snomax® INP measurements (all via freezing of suspensions) demonstrated discrepancies consistent with previous reports of the instability of its protein aggregates that appear to make it less suitable as a calibration INP at these temperatures. For Argentinian soil dust particles, there was excellent agreement across all measurement methods; measures ranged within 1 order of magnitude for INP number concentrations, active fractions and calculated active site densities over a 25 to 30 ∘C range and 5 to 8 orders of corresponding magnitude change in number concentrations. This was also the case for all temperatures warmer than −25 ∘C in Tunisian dust experiments. In contrast, discrepancies in measurements of INP concentrations or active site densities that exceeded 2 orders of magnitude across a broad range of temperature measurements found at temperatures warmer than −25 ∘C in a previous study were replicated for illite NX. Discrepancies also exceeded 2 orders of magnitude at temperatures of −20 to −25 ∘C for potassium feldspar (K-feldspar), but these coincided with the range of temperatures at which INP concentrations increase rapidly at approximately an order of magnitude per 2 ∘C cooling for K-feldspar. These few discrepancies did not outweigh the overall positive outcomes of the workshop activity, nor the future utility of this data set or future similar efforts for resolving remaining measurement issues. Measurements of the same materials were repeatable over the time of the workshop and demonstrated strong consistency with prior studies, as reflected by agreement of data broadly with parameterizations of different specific or general (e.g., soil dust) aerosol types. The divergent measurements of the INP activity of illite NX by direct versus post-processing methods were not repeated for other particle types, and the Snomax® data demonstrated that, at least for a biological INP type, there is no expected measurement bias between bulk collection and direct immediately processed freezing methods to as warm as −10 ∘C. Since particle size ranges were limited for this workshop, it can be expected that for atmospheric populations of INPs, measurement discrepancies will appear due to the different capabilities of methods for sampling the full aerosol size distribution, or due to limitations on achieving sufficient water supersaturations to fully capture immersion freezing in direct processing instruments. Overall, this workshop presents an improved picture of present capabilities for measuring INPs than in past workshops, and provides direction toward addressing remaining measurement issues

Particle surface area dependence of mineral dust in immersion freezing mode: investigations with freely suspended drops in an acoustic levitator and a vertical wind tunnel

The heterogeneous freezing temperatures of supercooled drops were measured using an acoustic levitator. This technique allows one to freely suspend single drops in the air without any wall contact. Heterogeneous nucleation by two types of illite (illite IMt1 and illite NX) and a montmorillonite sample was investigated in the immersion mode. Drops of 1 mm in radius were monitored by a video camera while cooled down to −28 °C to simulate freezing within the tropospheric temperature range. The surface temperature of the drops was contact-free, determined with an infrared thermometer; the onset of freezing was indicated by a sudden increase of the drop surface temperature. For comparison, measurements with one particle type (illite NX) were additionally performed in the Mainz vertical wind tunnel with drops of 340 μm radius freely suspended. Immersion freezing was observed in a temperature range between −13 and −26 °C as a function of particle type and particle surface area immersed in the drops. Isothermal experiments in the wind tunnel indicated that after the cooling stage freezing still proceeds, at least during the investigated time period of 30 s. The results were evaluated by applying two descriptions of heterogeneous freezing, the stochastic and the singular model. Although the wind tunnel results do not support the time-independence of the freezing process both models are applicable for comparing the results from the two experimental techniques

Comparative Study On Immersion Freezing Utilizing Single Droplet Levitation Methods

Immersion freezing experiments were performed utilizing two distinct single-droplet levitation methods. In the Mainz vertical wind tunnel (M-WT) supercooled droplets of 700 μm diameter were freely floated in a vertical air stream at constant temperatures ranging from −5 °C to −30 °C where heterogeneous freezing takes place. These investigations under isothermal conditions allow applying the stochastic approach to analyze and interpret the results in terms of the freezing or nucleation rate. In the Mainz acoustic levitator (M-AL) 2 mm diameter drops were levitated while their temperature was continuously cooling from +20 °C to −28 °C by adapting to the ambient temperature. Therefore, in this case the singular approach was used for analysis. From the experiments, the densities of ice nucleating active sites (INAS) were obtained as function of temperature. The direct comparison of the results from two different instruments indicates a shift of the freezing temperatures towards lower values that was material dependent. As ice nucleating particles, seven materials were investigated, two representatives of biological species (fibrous and microcrystalline cellulose), four mineral dusts (feldspar, illite NX, montmorillonite, and kaolinite), and natural Sahara dust. Based on detailed analysis of our results we determined a material dependent temperature correction factor for each investigated particle type. The analysis allowed further classifying the investigated materials as single- or multiple-component. From our experiences during the present synergetic studies, we listed a number of suggestions for future experiments regarding cooling rates, determination of the drop temperature, purity of the water used to produce the drops, and characterization of the ice nucleating material. The observed freezing temperature shift is significantly important not only for the intercomparison of ice nucleation instruments with different cooling rates but also for cloud model simulations with high speed ascents of air masses

Wintertime Airborne Measurements of Ice Nucleating Particles in the High Arctic: A Hint to a Marine, Biogenic Source for Ice Nucleating Particles

Ice nucleating particles (INPs) affect the radiative properties of cold clouds. Knowledge concerning their concentration above ground level and their potential sources is scarce. Here we present the first highly temperature resolved ice nucleation spectra of airborne samples from an aircraft campaign during late winter in 2018. Most INP spectra featured low concentration levels (<3 · 10−4 L−1 at −15°C). However, we also found INP concentrations of up to 1.8·10−2 L−1 at −15°C and freezing onsets as high as −7.5°C for samples mainly from the marine boundary layer. Shape and onset temperature of the ice nucleation spectra of those samples as well as heat sensitivity hint at biogenic INP. Colocated measurements additionally indicate a local marine influence rather than long‐range transport. Our results suggest that even in late winter above 80°N a local marine source for biogenic INP, which can efficiently nucleate ice at high temperatures, is present

Wintertime Airborne Measurements of Ice Nucleating Particles in the High Arctic: A Hint to a Marine, Biogenic Source for Ice Nucleating Particles

Ice nucleating particles (INPs) affect the radiative properties of cold clouds. Knowledge concerning their concentration above ground level and their potential sources is scarce. Here we present the first highly temperature resolved ice nucleation spectra of airborne samples from an aircraft campaign during late winter in 2018. Most INP spectra featured low concentration levels (<3 · 10−4 L−1 at −15°C). However, we also found INP concentrations of up to 1.8·10−2 L−1 at −15°C and freezing onsets as high as −7.5°C for samples mainly from the marine boundary layer. Shape and onset temperature of the ice nucleation spectra of those samples as well as heat sensitivity hint at biogenic INP. Colocated measurements additionally indicate a local marine influence rather than long-range transport. Our results suggest that even in late winter above 80°N a local marine source for biogenic INP, which can efficiently nucleate ice at high temperatures, is present