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.

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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.

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Icing conditions that contain supercooled large droplets (SLDs) represent a hazard for aviation. Due to their large inertia, SLDs impact behind the extent of aircraft ice protection systems where the developing ice accretion cannot be removed. At present, aircraft that are vulnerable to SLD icing need to avoid severe icing conditions in general, leading to increased operating costs. New American and European aviation regulations allow the passage through such conditions if the aircraft carries instruments that can detect the presence of SLDs. Upon detection, the pilots can exit the icing cloud before the situation becomes hazardous.
The mass of liquid water contained in an SLD is several orders of magnitude higher than the mass contained in a typical small cloud droplet. However, the number concentration of SLDs is much lower than that of small cloud droplets, consequently, it is challenging to detect SLDs with instruments. As of now, no instruments for the detection of SLD icing conditions are in use on commercial aircraft.
This thesis investigates a combination of two instruments for the detection of SLD icing conditions. The first instrument is the Nevzorov probe for the measurement of liquid and total water content and the second instrument is the Backscatter Cloud Probe with Polarization Detection (BCPD), a non-invasive laser backscatter probe that measures the size and shape of cloud particles between 2 and 42 µm. The Nevzorov probe used in this work carried a new, 12 mm diameter total water content sensor that was added to the instrument specifically for the measurement of SLD icing conditions. Both instruments, the Nevzorov probe and the BCPD, are first analyzed individually in icing wind tunnel tests. The findings from the tests show that the new 12 mm sensor of the Nevzorov probe captures SLDs effectively. No indication was found of SLD being incompletely evaporated due to splashing or of water being swept out of the cone. The collision efficiency of small droplets with the sensor is low and can be compensated with a correction derived in this work. Intensive atmospheric testing ensued the icing wind tunnel measurements. During measurements in Arctic clouds, it could be shown that the fraction of liquid and glaciated particles can be estimated from the BCPD. Measurements in the South of France were able to demonstrate that the detection and discrimination of SLD icing conditions is possible with the Nevzorov probe and the BCPD for SLD icing encounters that are sufficiently long and contain a high number of SLDs.
The results of this work allow future flight campaigns to use the 12 mm sensor of the Nevzorov probe and benefit from its capture efficiency and better sampling statistics. The comparisons of the Nevzorov probe to other instruments can help scientists choose suitable instrumentation for future icing wind tunnel and flight campaigns. Concerning the BCPD, a new method developed in this thesis to estimate the number of ice and water particles could, with small modifications, also be employed for other instruments that use polarization filters. For the detection and discrimination of SLD conditions, future work should focus on extending the sample area of the BCPD further outward from the aircraft skin to measure particle size distributions that are unaffected by the aircraft boundary layer. Furthermore, the false alarm rate of the system could be reduced by incorporating an instrument similar to the BCPD but with a larger size range and larger sample area for the direct detection of SLDs.@en

Observations show that the ice water content (IWC) in mixed-phase clouds (MPCs) tends to occur in clusters. However, it is not sufficiently understood which ice crystal formation and growth processes play a dominant role in IWC clustering in clouds. One important ice growth process is riming, which occurs when liquid water droplets freeze onto ice crystals upon contact. Here we use airborne measurements of MPCs at mid- and high-latitudes to investigate the spatial variability of ice clusters in clouds and how this variability is linked to riming. We use data from the IMPACTS (mid-latitudes) and the HALO-(AC)3 (high-latitudes) aircraft campaigns, where spatially and temporally colocated cloud radar and in situ measurements were collected. We derive riming and IWC by combining cloud radar and in situ measurements. Ice cluster scales in clouds are quantified using pair correlation functions.

During all analyzed flight segments, riming is responsible for 66 % and 63 % of the total IWC during IMPACTS and HALO-(AC)3, respectively. In mid-latitude MPCs, riming does not significantly change IWC cluster scales but increases the probability of cluster occurrence. In cold-air-outbreak MPCs observed during HALO-(AC)3, riming leads to additional in-cloud IWC clustering at spatial scales of 3–5 km due to the presence of mesoscale updraft features. An increased liquid water path might increase the effect, but it is not a necessary criterion. These results can be used to evaluate and constrain models' representations of MPCs.@en

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.

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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.

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Airborne in situ cloud measurements were carried out over the northern Fram Strait between Greenland and Svalbard in spring 2019 and summer 2020. In total, 811 min of low-level cloud observations were performed during 20 research flights above the sea ice and the open Arctic ocean with the Polar 5 research aircraft of the Alfred Wegener Institute. Here, we combine the comprehensive in situ cloud data to investigate the distributions of particle number concentration N, effective diameter Deff, and cloud water content CWC (liquid and ice) of Arctic clouds below 500 m altitude, measured at latitudes between 76 and 83∘ N. We developed a method to quantitatively derive the occurrence probability of their thermodynamic phase from the combination of microphysical cloud probe and Polar Nephelometer data. Finally, we assess changes in cloud microphysics and cloud phase related to ambient meteorological conditions in spring and summer and address effects of the sea ice and open-ocean surface conditions. We find median N from 0.2 to 51.7 cm−3 and about 2 orders of magnitude higher N for mainly liquid clouds in summer compared to ice and mixed-phase clouds measured in spring. A southerly flow from the sea ice in cold air outbreaks dominates cloud formation processes at temperatures mostly below −10 ∘C in spring, while northerly warm air intrusions favor the formation of liquid clouds at warmer temperatures in summer. Our results show slightly higher N in clouds over the sea ice compared to the open ocean, indicating enhanced cloud formation processes over the sea ice. The median CWC is higher in summer (0.16 g m−3) than in spring (0.06 g m−3), as this is dominated by the available atmospheric water content and the temperatures at cloud formation level. We find large differences in the particle sizes in spring and summer and an impact of the surface conditions, which modifies the heat and moisture fluxes in the boundary layer. By combining microphysical cloud data with thermodynamic phase information from the Polar Nephelometer, we find mixed-phase clouds to be the dominant thermodynamic cloud phase in spring, with a frequency of occurrence of 61 % over the sea ice and 66 % over the ocean. Pure ice clouds exist almost exclusively over the open ocean in spring, and in summer the cloud particles are most likely in the liquid water state.

The comprehensive low-level cloud data set will help us to better understand the role of clouds and their thermodynamic phase in the Arctic radiation budget and to assess the performance of global climate models in a region of the world with the strongest anthropogenic climate change.@en

Supercooled large droplet (SLD) icing can occur behind the protected surfaces of an aircraft and create severe aerodynamic disturbances, which represent a safety hazard for aviation. Liquid water content (LWC) measurements in icing conditions that contain SLDs require instruments that are able to sample unimodal and bimodal droplet size distributions with droplet diameters from 2 to 2000 µm. No standardized detection method exists for this task. A candidate instrument, which is currently used in icing wind tunnel (IWT) research, is the Nevzorov probe. In addition to the standard 8 mm total water content (TWC) collector cone, a novel instrument version also features a 12 mm diameter cone, which might be advantageous for collecting the large droplets characteristic of SLD conditions. In the scope of the two EU projects, SENSors and certifiable hybrid architectures for safer aviation in ICing Environment (SENS4ICE) and ICE GENESIS, we performed measurement campaigns in SLD icing conditions in IWTs in Germany, Austria and the USA. We obtained a comprehensive data set of measurements from the LWC sensor, the 8 mm cone sensor and the 12 mm cone sensor of the Nevzorov probe, and from the tunnel reference instrumentation. In combination with measurements of the particle size distribution, we experimentally derive a collision efficiency curve that is based on a suitable functional form for the new 12 mm cone for median volume diameters (MVDs) between 12 and 58 µm and wind tunnel speeds from 40 to 85 m s−1. Knowledge of this curve allows us to correct the LWC measurements of the 12 mm cone (LWC12) in particular for the inevitably high decrease in collision efficiency for small droplet diameters. In unimodal SLD conditions, with MVDs between 128 and 720 µm, LWC12 generally agrees within ±20 % with the tunnel LWC reference values from a WCM-2000 and an isokinetic probe. An increase in the difference between LWC12 and the WCM-2000 measurements at larger MVDs indicates better droplet collection properties of the 12 mm cone. Similarly, the favorable detector dimensions of the 12 mm cone explain a 7 % enhanced detection efficiency compared to the 8 mm cone; however this difference falls within the instrumental uncertainties. Data collected in various bimodal SLD conditions with MVDs between 16 and 534 µm and LWCs between 0.22 and 0.72 g m−3 also show an agreement within ±20 % between LWC12 and the tunnel LWC, which demonstrates the suitability of the Nevzorov sensor head with the 12 mm cone for measurements of LWC in Appendix O icing conditions.@en

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.

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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.

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