Supercooled large droplet (SLD) icing conditions threaten aviation safety. Two flight campaigns in SLD conditions were performed in February–March 2023 in the Great Lakes region and in April 2023 over France as part of the EU project SENS4ICE. This provides the opportunity to contrast and compare the observations of SLDs between these two locations and months. We present the altitudes, temperatures, number concentrations, liquid water contents, and cumulative mass distributions of the SLD conditions. During the North American flight campaign, SLD conditions were observed mostly in thick stratus clouds, and droplet size distributions were bimodal with an average median volume diameter (MVD) of 23 μm. Due to warmer ground temperatures in April, icing conditions during the European campaign occurred at higher altitudes; hence, predominantly midlevel clouds were sampled. The average MVD of SLD conditions was 45 μm. Our study suggests that the maritime origin of the European air masses, their likely low levels of pollution, and the associated low number of cloud condensation nuclei facilitated the formation of these SLD conditions with relatively large MVDs. The presented dataset can serve for model comparisons, process-oriented studies of icing conditions, and the validation of airborne sensors developed in the Sensors and Certifiable Hybrid Architectures for Safer Aviation in Icing Environment (SENS4ICE) project.

A comprehensive in-situ dataset of low-level Arctic clouds was collected in the Fram Strait during the HALO-(AC⁾³ campaign in spring 2022 using the research aircraft Polar 6. The clouds observed at altitudes below 1000 m were frequently in a mixed-phase state. We demonstrate that despite comparable optical properties, classic mixed-phase clouds (MPC) and mixed-phase haze (MPH) can be distinguished on the basis of their microphysical properties, with MPH observed about 8 times more frequently than MPC. While the thermodynamic phases of the particles within the MPH are similar to those in the MPC, the supercooled droplets observed in MPC are replaced by large (> 3 µm) wet aerosol particles in MPH. Furthermore, the particle number concentration measured in MPH is reduced by approximately 3 orders of magnitude compared to MPC. MPH is observed in subsaturated air with respect to water, suggesting that the small liquid particles are haze droplets and are in equilibrium below the activation threshold to form cloud droplets. Chemical analysis suggested that the haze particles contained significant amounts of sea salt. Additional in-situ measurements with an optical particle counter indicated that their number concentration was 2 times larger over the sea ice compared to the open ocean. Furthermore, measurements of the vertical distribution of the thermodynamic phases in low-level Arctic clouds revealed a characteristic structure, with a liquid regime frequently occurring at the top of the atmospheric boundary layer, followed by MPCs, and an MPH layer below. The findings from this study enhance our understanding of the microphysical composition of clouds in mixed-phase conditions.

The cloud condensation nuclei (CCN) concentrations greatly determine the vertical microphysical evolution and rain initiation of warm convective clouds. We investigated the vertical profile of aerosol particles large enough (diameter > 60 nm) to act as CCN in marine air masses over the Great Barrier Reef. Such data were collected during an aircraft research campaign in February 2024. The results show a strong relationship between the microphysical processes measured in the cloud and the aerosol properties measured at the same altitude. The number concentration of aerosol particles decreases significantly above cloud bases due to CCN activation into cloud droplets. For heights above the in-cloud rain initiation level, the aerosol concentrations decrease further due to the scavenging of particles by drizzle and raindrops. The Hoppel minimum in particle size distributions is observed up to the altitude at which the coagulation process intensifies. Furthermore, a tail of larger aerosol particles was measured above the altitudes of rain initiation. These results suggest that the vertical profile of aerosols measured in marine air masses is dominated by cloud processing. Plain text summary: Understanding the role of aerosol-cloud interactions is crucial information in accurately predicting the effects of climate change on the Great Barrier Reef (GBR). Characterizing the properties of aerosol particles found over the Reef is essential in determining their ability to act as cloud condensation nuclei (CCN). The evaporation of cloud droplets and raindrops represents an additional source that may influence the concentrations and sizes of aerosol. Here, we show that warm clouds dominate the vertical profiles of aerosol particles in the lower troposphere over the GBR. Our research shows that marine clouds work like a sink of aerosol particles found over the Reef. The cloud microphysical processes (activation of CCN into cloud droplets and the collision and coalescence processes) decrease the concentration of aerosol particles at the same altitude in the lower troposphere. Cloud processing develops the “Hoppel minima” or Hoppel minimum of the marine boundary layer aerosol size distributions as clouds evaporate. The Hoppel minimum is not observed in the particle size distributions above altitudes of intense coagulation processes. Above this level, the ultrafine particles dominate the aerosol concentrations.

Cold and dry Arctic air masses moving from sea ice southward over the open ocean rapidly heat up, moisten, and form clouds. Diabatic heating and moistening rates in such marine cold air outbreaks (CAOs) are key to understanding their dynamics. While state-of-the-art atmospheric reanalysis products are commonly used to estimate these rates, the uncertainties of these reanalysis data sets especially in 4-dimensional space required to calculate them remain largely unspecified. Therefore, we present an analysis based on actual quasi-Lagrangian observations, which offer direct insights into these processes and which were conducted during the HALO-(AC)3 Arctic airborne campaign. From the measurements during a case study of a CAO on 01 April 2022, a maximum moistening and diabatic heating larger than 0.25 g kg-1h-1 and 6 K h-1, respectively, were deduced. Clouds forming within 30 minutes of the off-ice drift then intensified the vertical mixing. In the later stages of the CAO, maximum increases of solar albedo of around 0.03-0.06 h-1 were observed. We suggest that such data collected in a dedicated Lagrangian framework will serve as invaluable input for the benchmarking of numerical weather-prediction models and modern reanalysis products.

Arctic air masses undergo intense transformations when moving southward from closed sea ice to warmer open waters in marine cold-Air outbreaks (CAOs). Due to the lack of measurements of diabatic heating and moisture uptake rates along CAO flows, studies often depend on atmospheric reanalysis output. However, the uncertainties connected to those datasets remain unclear. Here, we present height-resolved airborne observations of diabatic heating, moisture uptake, and cloud evolution measured in a quasi-Lagrangian manner. The investigated CAO was observed on 1 April 2022 during the HALO-(AC)3 campaign. Shortly after passing the sea-ice edge, maximum diabatic heating rates over 6ĝ€¯Kh-1 and moisture uptake over 0.3ĝ€¯gkg-1h-1 were measured near the surface. Clouds started forming and vertical mixing within the deepening boundary layer intensified. The quasi-Lagrangian observations are compared with the fifth-generation global reanalysis (ERA5) and the Copernicus Arctic Regional Reanalysis (CARRA). Compared to these observations, the mean absolute errors of ERA5 versus CARRA data are 14ĝ€¯% higher for air temperature over sea ice (1.14ĝ€¯K versus 1.00ĝ€¯K) and 62ĝ€¯% higher for specific humidity over ice-free ocean (0.112ĝ€¯gkg-1 versus 0.069ĝ€¯gkg-1). We relate these differences to issues with the representation of the marginal ice zone and corresponding surface fluxes in ERA5, as well as the cloud scheme producing excess liquid-bearing, precipitating clouds, which causes a too-dry marine boundary layer. CARRA's high spatial resolution and demonstrated higher fidelity towards observations make it a promising candidate for further studies on Arctic air mass transformations.

Riming is a key precipitation formation process in mixed-phase clouds which efficiently converts cloud liquid to ice water. Here, we present two methods to quantify riming of ice particles from airborne observations with the normalized rime mass, which is the ratio of rime mass to the mass of a size-equivalent spherical graupel particle. We use data obtained during the HALO-(AC)3 aircraft campaign, where two aircraft collected radar and in situ measurements that were closely spatially and temporally collocated over the Fram Strait west of Svalbard in spring 2022. The first method is based on an inverse optimal estimation algorithm for the retrieval of the normalized rime mass from a closure between cloud radar and in situ measurements during these collocated flight segments (combined method). The second method relies on in situ observations only, relating the normalized rime mass to optical particle shape measurements (in situ method). We find good agreement between both methods during collocated flight segments with median normalized rime masses of 0.024 and 0.021 (mean values of 0.035 and 0.033) for the combined and in situ method, respectively. Assuming that particles with a normalized rime mass smaller than 0.01 are unrimed, we obtain average rimed fractions of 88ĝ€¯% and 87ĝ€¯% over all collocated flight segments. Although in situ measurement volumes are in the range of a few cubic centimeters and are therefore much smaller than the radar volume (about 45ĝ€¯m footprint diameter at an altitude of 500ĝ€¯m above ground, with a vertical resolution of 5ĝ€¯m), we assume they are representative of the radar volume. When this assumption is not met due to less homogeneous conditions, discrepancies between the two methods result. We show the performance of the methods in a case study of a collocated segment of cold-air outbreak conditions and compare normalized rime mass results with meteorological and cloud parameters. We find that higher normalized rime masses correlate with streaks of higher radar reflectivity. The methods presented improve our ability to quantify riming from aircraft observations.

Despite their proven importance for the atmospheric radiative energy budget, the effect of cirrus on climate and the magnitude of their modification by human activity is not well quantified. Besides anthropogenic pollution sources on the ground, aviation has a large local effect on cirrus microphysical and radiative properties via the formation of contrails and their transition to contrail cirrus. To investigate the anthropogenic influence on natural cirrus, we compare the microphysical properties of cirrus measured at mid-latitude (ML) regions (<60 N) that are often affected by aviation and pollution with cirrus measured in the same season in comparatively pristine high latitudes (HLs; ≥60 N). The number concentration, effective diameter, and ice water content of the observed cirrus are derived from in situ measurements covering ice crystal sizes between 2 and 6400 μm collected during the CIRRUS-HL campaign (Cirrus in High Latitudes) in June and July 2021. We analyse the dependence of cirrus microphysical properties on altitude and latitude and demonstrate that the median ice number concentration is an order of magnitude larger in the measured mid-latitude cirrus, with 0.0086 cm^-3, compared to the high-latitude cirrus, with 0.001 cm^-3. Ice crystals in mid-latitude cirrus are on average smaller than in high-latitude cirrus, with a median effective diameter of 165 μm compared to 210 μm, and the median ice water content in mid-latitude cirrus is higher (0.0033 gm^-3) than in high-latitude cirrus (0.0019 gm^-3). In order to investigate the cirrus properties in relation to the region of formation, we combine the airborne observations with 10 d backward trajectories to identify the location of cirrus formation and the cirrus type, i.e. in situ or liquid origin cirrus, depending on whether there is only ice or also liquid water present in the cirrus history, respectively. The cirrus formed and measured at mid-latitudes (M-M) have a particularly high ice number concentration and low effective diameter. This is very likely a signature of contrails and contrail cirrus, which is often observed in the in situ origin cirrus type. In contrast, the largest effective diameter and lowest number concentration were found in the cirrus formed and measured at high latitudes (H-H) along with the highest relative humidity over ice (RHi). On average, in-cloud RHi was above saturation in all cirrus. While most of the H-H cirrus were of an in situ origin, the cirrus formed at mid-latitudes and measured at high latitudes (M-H) were mainly of liquid origin. A pristine Arctic background atmosphere with relatively low ice nuclei availability and the extended growth of few nucleated ice crystals may explain the observed RHi and size distributions. The M-H cirrus are a mixture of the properties of M-M and H-H cirrus (preserving some of the initial properties acquired at mid-latitudes and transforming under Arctic atmospheric conditions). Our analyses indicate that part of the cirrus found at high latitudes is actually formed at mid-latitudes and therefore affected by mid-latitude air masses, which have a greater anthropogenic influence.

During spring 2020, the COVID-19 pandemic caused massive reductions in emissions from industry and ground and airborne transportation. To explore the resulting atmospheric composition changes, we conducted the BLUESKY campaign with two research aircraft and measured trace gases, aerosols, and cloud properties from the boundary layer to the lower stratosphere. From 16 May to 9 June 2020, we performed 20 flights in the early COVID-19 lockdown phase over Europe and the Atlantic Ocean. We found up to 50% reductions in boundary layer nitrogen dioxide concentrations in urban areas from GOME-2B satellite data, along with carbon monoxide reductions in the pollution hot spots. We measured 20%-70% reductions in total reactive nitrogen, carbon monoxide, and fine mode aerosol concentration in profiles over German cities compared to a 10-yr dataset from passenger aircraft. The total aerosol mass was significantly reduced below 5 km altitude, and the organic aerosol fraction also aloft, indicative of decreased organic precursor gas emissions. The reduced aerosol optical thickness caused a perceptible shift in sky color toward the blue part of the spectrum (hence BLUESKY) and increased shortwave radiation at the surface. We find that the 80% decline in air traffic led to substantial reductions in nitrogen oxides at cruise altitudes, in contrail cover, and in resulting radiative forcing. The light extinction and depolarization by cirrus were also reduced in regions with substantially decreased air traffic. General circulation-chemistry model simulations indicate good agreement with the measurements when applying a reduced emission scenario. The comprehensive BLUESKY dataset documents the major impact of anthropogenic emissions on the atmospheric composition.

Sulfur compounds in the upper troposphere and lower stratosphere (UTLS) impact the atmosphere radiation budget, either directly as particles or indirectly as precursor gas for new particle formation. In situ measurements in the UTLS are rare but are important to better understand the impact of the sulfur budget on climate. The BLUESKY mission in May and June 2020 explored an unprecedented situation. (1) The UTLS experienced extraordinary dry conditions in spring 2020 over Europe, in comparison to previous years, and (2) the first lockdown of the COVID-19 pandemic caused major emission reductions from industry, ground, and airborne transportation. With the two research aircraft HALO and Falcon, 20 flights were conducted over central Europe and the North Atlantic to investigate the atmospheric composition with respect to trace gases, aerosol, and clouds. Here, we focus on measurements of sulfur dioxide (SO2) and particulate sulfate (SO42-) in the altitude range of 8 to 14.5gkm which show unexpectedly enhanced mixing ratios of SO2 in the upper troposphere and of SO42- in the lowermost stratosphere. In the UT, we find SO2 mixing ratios of (0.07±0.01)gppb, caused by the remaining air traffic, and reduced SO2 sinks due to low OH and low cloud fractions and to a minor extent by uplift from boundary layer sources. Particulate sulfate showed elevated mixing ratios of up to 0.33gppb in the LS. We suggest that the eruption of the volcano Raikoke in June 2019, which emitted about 1gTggSO2 into the stratosphere in northern midlatitudes, caused these enhancements, in addition to Siberian and Canadian wildfires and other minor volcanic eruptions. Our measurements can help to test models and lead to new insights in the distribution of sulfur compounds in the UTLS, their sources, and sinks. Moreover, these results can contribute to improving simulations of the radiation budget in the UTLS with respect to sulfur effects.