Explore the vast range of titles available.

Global sulfate production plays a key role in aerosol radiative forcing; more than half of this production occurs in clouds. We found that sulfur dioxide oxidation catalyzed by natural transition metal ions is the dominant in-cloud oxidation pathway. The pathway was observed to occur primarily on coarse mineral dust, so the sulfate produced will have a short lifetime and little direct or indirect climatic effect. Taking this into account will lead to large changes in estimates of the magnitude and spatial distribution of aerosol forcing. Therefore, this oxidation pathway-which is currently included in only one of the 12 major global climate models-will have a significant impact on assessments of current and future climate.

Cloud water samples were taken in September/October 2010 at Mt. Schmücke in a rural, forested area in Germany during the Lagrange-type Hill Cap Cloud Thuringia 2010 (HCCT-2010) cloud experiment. Besides bulk collectors, a three-stage and a five-stage collector were applied and samples were analysed for inorganic ions (SO42−,NO3−, NH4+, Cl−, Na+, Mg2+, Ca2+, K+), H2O2 (aq), S(IV), and dissolved organic carbon (DOC). Campaign volume-weighted mean concentrations were 191, 142, and 39 µmol L−1 for ammonium, nitrate, and sulfate respectively, between 4 and 27 µmol L−1 for minor ions, 5.4 µmol L−1 for H2O2 (aq), 1.9 µmol L−1 for S(IV), and 3.9 mgC L−1 for DOC. The concentrations compare well to more recent European cloud water data from similar sites. On a mass basis, organic material (as DOC × 1.8) contributed 20–40 % (event means) to total solute concentrations and was found to have non-negligible impact on cloud water acidity. Relative standard deviations of major ions were 60–66 % for solute concentrations and 52–80 % for cloud water loadings (CWLs). The similar variability of solute concentrations and CWLs together with the results of back-trajectory analysis and principal component analysis, suggests that concentrations in incoming air masses (i.e. air mass history), rather than cloud liquid water content (LWC), were the main factor controlling bulk solute concentrations for the cloud studied. Droplet effective radius was found to be a somewhat better predictor for cloud water total ionic content (TIC) than LWC, even though no single explanatory variable can fully describe TIC (or solute concentration) variations in a simple functional relation due to the complex processes involved. Bulk concentrations typically agreed within a factor of 2 with co-located measurements of residual particle concentrations sampled by a counterflow virtual impactor (CVI) and analysed by an aerosol mass spectrometer (AMS), with the deviations being mainly caused by systematic differences and limitations of the approaches (such as outgassing of dissolved gases during residual particle sampling). Scavenging efficiencies (SEs) of aerosol constituents were 0.56–0.94, 0.79–0.99, 0.71–98, and 0.67–0.92 for SO42−, NO3−, NH4+, and DOC respectively when calculated as event means with in-cloud data only. SEs estimated using data from an upwind site were substantially different in many cases, revealing the impact of gas-phase uptake (for volatile constituents) and mass losses across Mt. Schmücke likely due to physical processes such as droplet scavenging by trees and/or entrainment. Drop size-resolved cloud water concentrations of major ions SO42−, NO3−, and NH4+ revealed two main profiles: decreasing concentrations with increasing droplet size and “U” shapes. In contrast, profiles of typical coarse particle mode minor ions were often increasing with increasing drop size, highlighting the importance of a species' particle concentration size distribution for the development of size-resolved solute concentration patterns. Concentration differences between droplet size classes were typically < 2 for major ions from the three-stage collector and somewhat more pronounced from the five-stage collector, while they were much larger for minor ions. Due to a better separation of droplet populations, the five-stage collector was capable of resolving some features of solute size dependencies not seen in the three-stage data, especially sharp concentration increases (up to a factor of 5–10) in the smallest droplets for many solutes.

Ice particle residuals (IRs) and the total aerosol particle population were sampled in parallel during mixed-phase cloud events at the high-altitude research station Jungfraujoch in January–February 2017. Particles were sampled behind an ice-selective counterflow impactor (Ice-CVI) for IRs and a heated total inlet for the total aerosol particles. A dilution set-up was used to collect total particles with the same sampling duration as for IRs to prevent overloading of the substrates. About 4000 particles from 10 Ice-CVI samples (from 7 days of cloud events at temperatures at the site between −10 and −18 ∘C) were analysed and classified with operator-controlled scanning electron microscopy. Contamination particles (identified by their chemical composition), most likely originating from abrasion in the Ice-CVI and collection of secondary ice, were excluded from further analysis. Approximately 3000 total aerosol particles (IRs and interstitial particles) from 5 days in clouds were also analysed. Enrichment and depletion of the different particle groups (within the IR fraction relative to the total aerosol reservoir) are presented as an odds ratio relative to alumosilicate (particles only consisting of Al, Si, and O), which was chosen as reference due to the large enrichment of this group relative to total aerosol and the relatively high number concentration of this group in both total aerosol and the IR samples. Complex secondary particles and soot are the major particle groups in the total aerosol samples but are not found in the IR fraction and are hence strongly depleted. C-rich particles (most likely organic particles) showed a smaller enrichment compared to aluminosilicates by a factor of ∼20. The particle groups with enrichment similar to aluminosilicate are silica, Fe aluminosilicates, Ca-rich particles, Ca sulfates, sea-salt-containing particles, and metal/metal oxide. Other aluminosilicates – consisting of variable amounts of Na, K, Ca, Si, Al, O, Ti, and Fe – are somewhat more enriched (factor ∼2) and Pb-rich particles are more (factor ∼8) enriched than aluminosilicates. None of the sampled IR groups showed a temperature or size dependence in respect to ice activity, which might be due to the limited sampling temperature interval and the similar size of the particles. Footprint plots and wind roses could explain the different total aerosol composition in one sample (carbonaceous particle emission from the urban/industrial area of Po Valley), but this did not affect the IR composition. Taking into account the relative abundance of the particle groups in total aerosol and the ice nucleation ability, we found that silica, aluminosilicates, and other aluminosilicates were the most important ice particle residuals at Jungfraujoch during the mixed-phase cloud events in winter 2017.

The Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) campaign was carried out north-west of Svalbard (Norway) between 23 May and 6 June 2017. The objective of ACLOUD was to study Arctic boundary layer and mid-level clouds and their role in Arctic amplification. Two research aircraft (Polar 5 and 6) jointly performed 22 research flights over the transition zone between open ocean and closed sea ice. Both aircraft were equipped with identical instrumentation for measurements of basic meteorological parameters, as well as for turbulent and radiative energy fluxes. In addition, on Polar 5 active and passive remote sensing instruments were installed, while Polar 6 operated in situ instruments to characterize cloud and aerosol particles as well as trace gases. A detailed overview of the specifications, data processing, and data quality is provided here. It is shown that the scientific analysis of the ACLOUD data benefits from the coordinated operation of both aircraft. By combining the cloud remote sensing techniques operated on Polar 5, the synergy of multi-instrument cloud retrieval is illustrated. The remote sensing methods were validated using truly collocated in situ and remote sensing observations. The data of identical instruments operated on both aircraft were merged to extend the spatial coverage of mean atmospheric quantities and turbulent and radiative flux measurement. Therefore, the data set of the ACLOUD campaign provides comprehensive in situ and remote sensing observations characterizing the cloudy Arctic atmosphere. All processed, calibrated, and validated data are published in the World Data Center PANGAEA as instrument-separated data subsets (Ehrlich et al., 2019b, https://doi.org/10.1594/PANGAEA.902603).

Clouds play an important role in Arctic amplification. This term represents the recently observed enhanced warming of the Arctic relative to the global increase of near-surface air temperature. However, there are still important knowledge gaps regarding the interplay between Arctic clouds and aerosol particles, and surface properties, as well as turbulent and radiative fluxes that inhibit accurate model simulations of clouds in the Arctic climate system. In an attempt to resolve this so-called Arctic cloud puzzle, two comprehensive and closely coordinated field studies were conducted: the Arctic Cloud Observations Using Airborne Measurements during Polar Day (ACLOUD) aircraft campaign and the Physical Feedbacks of Arctic Boundary Layer, Sea Ice, Cloud and Aerosol (PASCAL) ice breaker expedition. Both observational studies were performed in the framework of the German Arctic Amplification: Climate Relevant Atmospheric and Surface Processes, and Feedback Mechanisms (AC) project. They took place in the vicinity of Svalbard, Norway, in May and June 2017. ACLOUD and PASCAL explored four pieces of the Arctic cloud puzzle: cloud properties, aerosol impact on clouds, atmospheric radiation, and turbulent dynamical processes. The two instrumented Polar 5 and Polar 6 aircraft; the icebreaker Research Vessel (R/V) Polarstern; an ice floe camp including an instrumented tethered balloon; and the permanent ground-based measurement station at Ny-Ålesund, Svalbard, were employed to observe Arctic low- and mid-level mixed-phase clouds and to investigate related atmospheric and surface processes. The Polar 5 aircraft served as a remote sensing observatory examining the clouds from above by downward-looking sensors; the Polar 6 aircraft operated as a flying in situ measurement laboratory sampling inside and below the clouds. Most of the collocated Polar 5/6 flights were conducted either above the R/V Polarstern or over the Ny-Ålesund station, both of which monitored the clouds from below using similar but upward-looking remote sensing techniques as the Polar 5 aircraft. Several of the flights were carried out underneath collocated satellite tracks. The paper motivates the scientific objectives of the ACLOUD/PASCAL observations and describes the measured quantities, retrieved parameters, and the applied complementary instrumentation. Furthermore, it discusses selected measurement results and poses critical research questions to be answered in future papers analyzing the data from the two field campaigns.

Atmospheric ice-nucleating particle (INP) concentration data from the free troposphere are sparse but urgently needed to understand vertical transport processes of INPs and their influence on cloud formation and properties. Here, we introduce the new High-volume flow aERosol particle filter sAmpler (HERA) which was specially developed for installation on research aircraft and subsequent offline INP analysis. HERA is a modular system consisting of a sampling unit and a powerful pump unit, and it has several features which were integrated specifically for INP sampling. Firstly, the pump unit enables sampling at flow rates exceeding 100 L min−1, which is well above typical flow rates of aircraft INP sampling systems described in the literature (∼ 10 L min−1). Consequently, required sampling times to capture rare, high-temperature INPs (≥ −15 ∘C) are reduced in comparison to other systems, and potential source regions of INPs can be confined more precisely. Secondly, the sampling unit is designed as a seven-way valve, enabling switching between six filter holders and a bypass with one filter being sampled at a time. In contrast to other aircraft INP sampling systems, the valve position is remote-controlled via software so that manual filter changes during flight are eliminated and the potential for sample contamination is decreased. This design is compatible with a high degree of automation, i.e., triggering filter changes depending on parameters like flight altitude, geographical location, temperature, or time. In addition to presenting the design and principle of operation of HERA, this paper describes laboratory characterization experiments with size-selected test substances, i.e., SNOMAX® and Arizona Test Dust. The particles were sampled on filters with HERA, varying either particle diameter (300 to 800 nm) or flow rate (10 to 100 L min−1) between experiments. The subsequent offline INP analysis showed good agreement with literature data and comparable sampling efficiencies for all investigated particle sizes and flow rates. Furthermore, the collection efficiency of atmospheric INPs in HERA was compared to a straightforward filter sampler and good agreement was found. Finally, results from the first campaign of HERA on the High Altitude and LOng range research aircraft (HALO) demonstrate the functionality of the new system in the context of aircraft application.

Concurrent in situ analyses of interstitial aerosol and cloud droplet residues have been conducted at the Schmücke mountain site during the Hill Cap Cloud Thuringia campaign in central Germany in September and October 2010. Cloud droplets were sampled from warm clouds (temperatures between −3 and +16 °C) by a counterflow virtual impactor and the submicron-sized residues were analyzed by a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), while the interstitial aerosol composition was measured by an high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). During cloud-free periods, the submicron out-of-cloud aerosol was analyzed using both instruments, allowing for intercomparison between the two instruments. Further instrumentation included black carbon measurements and optical particle counters for the aerosol particles as well as optical sizing instrumentation for the cloud droplets. The results show that, under cloud conditions, on average 85 % of the submicron aerosol mass partitioned into the cloud liquid phase. Scavenging efficiencies of nitrate, ammonium, sulfate, and organics ranged between 60 and 100 %, with nitrate having, in general, the highest values. For black carbon, the scavenging efficiency was markedly lower (about 24 %). The nitrate and ammonium mass fractions were found to be markedly enhanced in cloud residues, indicating uptake of gaseous nitric acid and ammonia into the aqueous phase. This effect was found to be temperature dependent: at lower temperatures, the nitrate and ammonium mass fractions in the residues were higher. Also, the oxidation state of the organic matter in cloud residues was found to be temperature dependent: the O : C ratio was lower at higher temperatures. A possible explanation for this observation is a more effective uptake and/or higher concentrations of low-oxidized water-soluble volatile organic compounds, possibly of biogenic origin, at higher temperatures. Organic nitrates were observed in cloud residuals as well as in the out-of-cloud aerosol, but no indication of a preferred partitioning of organic nitrates into the aqueous phase or into the gas phase was detected. Assuming the uptake of nitric acid and ammonia in cloud droplets will be reversible, it will lead to a redistribution of nitrate and ammonium among the aerosol particles, leading to more uniform, internally mixed particles after several cloud passages.

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.

In situ single particle analysis of ice particle residuals (IPRs) and out-of-cloud aerosol particles was conducted by means of laser ablation mass spectrometry during the intensive INUIT-JFJ/CLACE campaign at the high alpine research station Jungfraujoch (3580 m a.s.l.) in January–February 2013. During the 4-week campaign more than 70 000 out-of-cloud aerosol particles and 595 IPRs were analyzed covering a particle size diameter range from 100 nm to 3 µm. The IPRs were sampled during 273 h while the station was covered by mixed-phase clouds at ambient temperatures between −27 and −6 °C. The identification of particle types is based on laboratory studies of different types of biological, mineral and anthropogenic aerosol particles. The outcome of these laboratory studies was characteristic marker peaks for each investigated particle type. These marker peaks were applied to the field data. In the sampled IPRs we identified a larger number fraction of primary aerosol particles, like soil dust (13 ± 5 %) and minerals (11 ± 5 %), in comparison to out-of-cloud aerosol particles (2.4 ± 0.4 and 0.4 ± 0.1 %, respectively). Additionally, anthropogenic aerosol particles, such as particles from industrial emissions and lead-containing particles, were found to be more abundant in the IPRs than in the out-of-cloud aerosol. In the out-of-cloud aerosol we identified a large fraction of aged particles (31 ± 5 %), including organic material and secondary inorganics, whereas this particle type was much less abundant (2.7 ± 1.3 %) in the IPRs. In a selected subset of the data where a direct comparison between out-of-cloud aerosol particles and IPRs in air masses with similar origin was possible, a pronounced enhancement of biological particles was found in the IPRs.

Between 1 September and 4 October 2014, a combined airborne and ground-based measurement campaign was conducted to study tropical deep convective clouds over the Brazilian Amazon rain forest. The new German research aircraft, High Altitude and Long Range Research Aircraft (HALO), a modified Gulfstream G550, and extensive ground-based instrumentation were deployed in and near Manaus (State of Amazonas). The campaign was part of the German–Brazilian Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON–CHUVA) venture to quantify aerosol–cloud–precipitation interactions and their thermodynamic, dynamic, and radiative effects by in situ and remote sensing measurements over Amazonia. The ACRIDICON–CHUVA field observations were carried out in cooperation with the second intensive operating period of Green Ocean Amazon 2014/15 (GoAmazon2014/5). In this paper we focus on the airborne data measured on HALO, which was equipped with about 30 in situ and remote sensing instruments for meteorological, trace gas, aerosol, cloud, precipitation, and spectral solar radiation measurements. Fourteen research flights with a total duration of 96 flight hours were performed. Five scientific topics were pursued: 1) cloud vertical evolution and life cycle (cloud profiling), 2) cloud processing of aerosol particles and trace gases (inflow and outflow), 3) satellite and radar validation (cloud products), 4) vertical transport and mixing (tracer experiment), and 5) cloud formation over forested/deforested areas. Data were collected in near-pristine atmospheric conditions and in environments polluted by biomass burning and urban emissions. The paper presents a general introduction of the ACRIDICON–CHUVA campaign (motivation and addressed research topics) and of HALO with its extensive instrument package, as well as a presentation of a few selected measurement results acquired during the flights for some selected scientific topics.