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Global warming is amplified in the Arctic. However, numerical models struggle to represent key processes that determine Arctic weather and climate. To collect data that help to constrain the models, the HALO–(𝒜𝒞)3 aircraft campaign was conducted over the Norwegian and Greenland seas, the Fram Strait, and the central Arctic Ocean in March and April 2022. The campaign focused on one specific challenge posed by the models, namely the reasonable representation of transformations of air masses during their meridional transport into and out of the Arctic via northward moist- and warm-air intrusions (WAIs) and southward marine cold-air outbreaks (CAOs). Observations were made over areas of open ocean, the marginal sea ice zone, and the central Arctic sea ice. Two low-flying and one long-range, high-altitude research aircraft were flown in colocated formation whenever possible. To follow the air mass transformations, a quasi-Lagrangian flight strategy using trajectory calculations was realized, enabling us to sample the same moving-air parcels twice along their trajectories. Seven distinct WAI and 12 CAO cases were probed. From the quasi-Lagrangian measurements, we have quantified the diabatic heating/cooling and moistening/drying of the transported air masses. During CAOs, maximum values of 3 K h−1 warming and 0.3 g kg−1 h−1 moistening were obtained below 1 km altitude. From the observations of WAIs, diabatic cooling rates of up to 0.4 K h−1 and a moisture loss of up to 0.1 g kg−1 h−1 from the ground to about 5.5 km altitude were derived. Furthermore, the development of cloud macrophysical (cloud-top height and horizontal cloud cover) and microphysical (liquid water path, precipitation, and ice index) properties along the southward pathways of the air masses were documented during CAOs, and the moisture budget during a specific WAI event was estimated. In addition, we discuss the statistical frequency of occurrence of the different thermodynamic phases of Arctic low-level clouds, the interaction of Arctic cirrus clouds with sea ice and water vapor, and the characteristics of microphysical and chemical properties of Arctic aerosol particles. Finally, we provide a proof of concept to measure mesoscale divergence and subsidence in the Arctic using data from dropsondes released during the flights.

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.

Vertical profiles of the mass concentration of black carbon (BC) were measured at altitudes up to 5 km during the PAMARCMiP (Polar Airborne Measurements and Arctic Regional Climate Model simulation Project) aircraft-based field experiment conducted around the northern Greenland Sea (Fram Strait) during March and April 2018 from operation base Station Nord (81.6∘ N, 16.7∘ W). Median BC mass concentrations in individual altitude ranges were 7–18 ng m−3 at standard temperature and pressure at altitudes below 4.5 km. These concentrations were systematically lower than previous observations in the Arctic in spring, conducted by ARCTAS-A in 2008 and NETCARE in 2015, and similar to those observed during HIPPO3 in 2010. Column amounts of BC for altitudes below 5 km in the Arctic (>66.5∘ N; COLBC), observed during the ARCTAS-A and NETCARE experiments, were higher by factors of 4.2 and 2.7, respectively, than those of the PAMARCMiP experiment. These differences could not be explained solely by the different locations of the experiments. The year-to-year variation of COLBC values generally corresponded to that of biomass burning activities in northern midlatitudes over western and eastern Eurasia. Furthermore, numerical model simulations estimated the year-to-year variation of contributions from anthropogenic sources to be smaller than 30 %–40 %. These results suggest that the year-to-year variation of biomass burning activities likely affected BC amounts in the Arctic troposphere in spring, at least in the years examined in this study. The year-to-year variations in BC mass concentrations were also observed at the surface at high Arctic sites Ny-Ålesund and Utqiaġvik (formerly known as Barrow, the location of Barrow Atmospheric Baseline Observatory), although their magnitudes were slightly lower than those in COLBC. Numerical model simulations in general successfully reproduced the observed COLBC values for PAMARCMiP and HIPPO3 (within a factor of 2), whereas they markedly underestimated the values for ARCTAS-A and NETCARE by factors of 3.7–5.8 and 3.3–5.0, respectively. Because anthropogenic contributions account for nearly all of the COLBC (82 %–98 %) in PAMARCMiP and HIPPO3, the good agreement between the observations and calculations for these two experiments suggests that anthropogenic contributions were generally well reproduced. However, the significant underestimations of COLBC for ARCTAS-A and NETCARE suggest that biomass burning contributions were underestimated. In this study, we also investigated plumes with enhanced BC mass concentrations, which were affected by biomass burning emissions, observed at 5 km altitude. Interestingly, the mass-averaged diameter of BC (core) and the shell-to-core diameter ratio of BC-containing particles in the plumes were generally not very different from those in other air samples, which were considered to be mostly aged anthropogenic BC. These observations provide a useful basis to evaluate numerical model simulations of the BC radiative effect in the Arctic region in spring.

After aerosol deposition from the atmosphere, black carbon (BC) takes part in the snow albedo feedback contributing to the modification of the Arctic radiative budget. With the initial goal of quantifying the concentration of BC in the Arctic snow and subsequent climatic impacts, snow samples were collected during the research vessel (R/V) Polarstern expedition of PASCAL (Physical Feedbacks of Arctic Boundary Layer, Sea Ice, Cloud and Aerosol; Polarstern cruise 106) in the sea-ice-covered Fram Strait in early summer 2017. The refractory BC (rBC) content was then measured in the laboratory of the Alfred Wegener Institute with the single particle soot photometer (SP2). Based on the strong observational correlations between both rBC concentration and rBC diameter with snow salinity, we hypothesize a salt-induced matrix effect interfering with the SP2 analysis. This paper evaluates the impact of sea salt, based on the measurement of electrical conductivity (κ) in water samples, on rBC measurements made with a SP2 nebulizer technique. Under realistic salinity conditions, laboratory experiments indicated a dramatic six-fold reduction in observed rBC concentration with increasing salinity. In the salinity conditions tested in the present work (salt concentration below 0.4 g L−1) the impact of salt on the nebulization of water droplets might be negligible. However, the SP2 mass detection efficiency systematically decreased with increasing salinity, with the smaller rBC particles being preferentially undetected. The high concentration of suspended salt particles and the formation of thick salt coatings on rBC cores caused problems in the SP2 analog-to-digital conversion of the signal and incandescence quenching, respectively. Changes to the signal acquisition parameters and the laser power of the SP2 improved the mass detection efficiency, which, nonetheless, stayed below unity. The present work provides evidence that a high concentration of sea salt undermines the quantification of rBC in snow performed with the SP2 nebulizer system described here. This interference has not been previously reported and might affect the future such analysis of rBC particles in snow collected, especially over sea ice or coastal regions strongly affected by sea salt deposition.

Immersion freezing experiments were performed utilizing two distinct single-droplet levitation methods. In the Mainz vertical wind tunnel, supercooled droplets of 700 µm diameter were freely floated in a vertical airstream at constant temperatures ranging from −5 to −30 ∘C, where heterogeneous freezing takes place. These investigations under isothermal conditions allow the application of the stochastic approach to analyze and interpret the results in terms of the freezing or nucleation rate. In the Mainz acoustic levitator, 2 mm diameter drops were levitated while their temperature was continuously cooling from +20 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 nucleation active sites were obtained as a function of temperature. The direct comparison of the results from two different instruments indicates a shift in the mean freezing temperatures of the investigated drops 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 parameter for calculating the freezing-temperature shift due to a change in cooling rate for each investigated particle type. The analysis allowed further classification of the investigated materials to be described by a single- or a multiple-component approach. 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 for the intercomparison of ice nucleation instruments with different cooling rates.

We analyse aerosol particle composition measurements from five research missions between 2014 and 2018 to assess the meridional extent of particles containing meteoric material in the upper troposphere and lower stratosphere (UTLS). Measurements from the Jungfraujoch mountaintop site and a low-altitude aircraft mission show that meteoric material is also present within middle- and lower-tropospheric aerosol but within only a very small proportion of particles. For both the UTLS campaigns and the lower- and mid-troposphere observations, the measurements were conducted with single-particle laser ablation mass spectrometers with bipolar-ion detection, which enabled us to measure the chemical composition of particles in a diameter range of approximately 150 nm to 3 µm. The five UTLS aircraft missions cover a latitude range from 15 to 68∘ N, altitudes up to 21 km, and a potential temperature range from 280 to 480 K. In total, 338 363 single particles were analysed, of which 147 338 were measured in the stratosphere. Of these total particles, 50 688 were characterized by high abundances of magnesium and iron, together with sulfuric ions, the vast majority (48 610) in the stratosphere, and are interpreted as meteoric material immersed or dissolved within sulfuric acid. It must be noted that the relative abundance of such meteoric particles may be overestimated by about 10 % to 30 % due to the presence of pure sulfuric acid particles in the stratosphere which are not detected by the instruments used here. Below the tropopause, the observed fraction of the meteoric particle type decreased sharply with 0.2 %–1 % abundance at Jungfraujoch, and smaller abundances (0.025 %–0.05 %) were observed during the lower-altitude Canadian Arctic aircraft measurements. The size distribution of the meteoric sulfuric particles measured in the UTLS campaigns is consistent with earlier aircraft-based mass-spectrometric measurements, with only 5 %–10 % fractions in the smallest particles detected (200–300 nm diameter) but with substantial (> 40 %) abundance fractions for particles from 300–350 up to 900 nm in diameter, suggesting sedimentation is the primary loss mechanism. In the tropical lower stratosphere, only a small fraction (< 10 %) of the analysed particles contained meteoric material. In contrast, in the extratropics the observed fraction of meteoric particles reached 20 %–40 % directly above the tropopause. At potential temperature levels of more than 40 K above the thermal tropopause, particles containing meteoric material were observed in much higher relative abundances than near the tropopause, and, at these altitudes, they occurred at a similar abundance fraction across all latitudes and seasons measured. Above 440 K, the observed fraction of meteoric particles is above 60 % at latitudes between 20 and 42∘ N. Meteoric smoke particles are transported from the mesosphere into the stratosphere within the winter polar vortex and are subsequently distributed towards low latitudes by isentropic mixing, typically below a potential temperature of 440 K. By contrast, the findings from the UTLS measurements show that meteoric material is found in stratospheric aerosol particles at all latitudes and seasons, which suggests that either isentropic mixing is effective also above 440 K or that meteoric fragments may be the source of a substantial proportion of the observed meteoric material.

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 

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.