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This study presents in situ aircraft measurements of Saharan mineral dust transported over the western Mediterranean basin in June–July 2013 during the ChArMEx/ADRIMED (the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) airborne campaign. Dust events differing in terms of source region (Algeria, Tunisia and Morocco), time of transport (1–5 days) and height of transport were sampled. Mineral dust were transported above the marine boundary layer, which conversely was dominated by pollution and marine aerosols. The dust vertical structure was extremely variable and characterized by either a single layer or a more complex and stratified structure with layers originating from different source regions. Mixing of mineral dust with pollution particles was observed depending on the height of transport of the dust layers. Dust layers carried a higher concentration of pollution particles below 3 km above sea level (a.s.l.) than above 3 km a.s.l., resulting in a scattering Ångström exponent up to 2.2 below 3 km a.s.l. However, the optical properties of the dust plumes remained practically unchanged with respect to values previously measured over source regions, regardless of the altitude. Moderate absorption of light by the dust plumes was observed with values of aerosol single scattering albedo at 530 nm ranging from 0.90 to 1.00. Concurrent calculations from the aerosol chemical composition revealed a negligible contribution of pollution particles to the absorption properties of the dust plumes that was due to a low contribution of refractory black carbon in regards to the fraction of dust and sulfate particles. This suggests that, even in the presence of moderate pollution, likely a persistent feature in the Mediterranean, the optical properties of the dust plumes could be assumed similar to those of native dust in radiative transfer simulations, modelling studies and satellite retrievals over the Mediterranean. Measurements also showed that the coarse mode of mineral dust was conserved even after 5 days of transport in the Mediterranean, which contrasts with the gravitational depletion of large particles observed during the transport of dust plumes over the Atlantic. Simulations with the WRF mesoscale meteorological model highlighted a strong vertical turbulence within the dust layers that could prevent deposition of large particles during their atmospheric transport. This has important implications for the dust radiative effects due to surface dimming, atmospheric heating and cloud formation. The results presented here add to the observational data set necessary for evaluating the role of mineral dust on the regional climate and rainfall patterns in the western Mediterranean basin and understanding their atmospheric transport at global scale.

We have studied the hydration of sulfuric acid – ammonia and sulfuric acid – dimethylamine clusters using quantum chemistry. We calculated the formation energies and thermodynamics for clusters of one ammonia or one dimethylamine molecule together with 1–2 sulfuric acid and 0–5 water molecules. The results indicate that dimethylamine enhances the addition of sulfuric acid to the clusters much more efficiently than ammonia when the number of water molecules in the cluster is either zero, or greater than two. Further hydrate distribution calculations reveal that practically all dimethylamine-containing two-acid clusters will remain unhydrated in tropospherically relevant circumstances, thus strongly suggesting that dimethylamine assists atmospheric sulfuric acid nucleation much more effectively than ammonia.

There is growing evidence that marine microorganisms may influence cloud cover over the ocean through their impact on sea spray and trace gas emissions, further forming cloud droplets or ice crystals. However, evidence of a robust causal relationship based on observations is still pending. In this study, we use 4 years of multi‐instrument satellite data to segregate low‐level clouds into ice‐containing and liquid‐water clouds to obtain clear relationships between cloud types and ocean biological tracers, especially with nanophytoplankton cell abundances. Results suggest that microorganisms may be involved in compensating effects on cloud properties, increasing the frequency of occurrence of warm‐liquid clouds, and decreasing the occurrence of ice‐containing clouds in most regions during springtime. The relationships observed in most regions do not apply to the South Pacific Ocean in the 40°S–50°S latitude band. These results shed light on overlooked potential compensating effects of ocean microorganisms on cloud cover. Plain Language Summary Climate is governed by interactions between the ocean and the atmosphere. While physical interactions such as exchanges of heat and water vapor are fairly well understood, the role of biology, that is, the living marine microorganisms, on atmospheric processes, is a lot more complex. For instance, marine microorganisms may influence the number and the chemical composition of sea sprays and also emit trace gasses that will form tiny particles. Sea sprays and newly formed particles can then serve as nuclei on which cloud droplets or ice crystals form, therefore influencing cloud properties and climate. These chains of processes are theoretical, and there are few clear linkages between ocean biology and cloud properties derived from observational data. This study uses new satellite retrievals to establish relationships between cloud phase occurrence (ice, warm‐liquid, mixed‐phase or supercooled‐liquid clouds) and the biological activity of the ocean in different regions of the southern ocean. For a given month, locations of higher abundance of phytoplankton corresponds to a higher warm‐liquid cloud cover but lower ice cloud cover. These results suggest compensating effects of marine microorganisms on cloud lifetime via their potential to impact the formation of particles able to become water droplets or ice crystals. Key Points Nanophytoplankton biomass shows more relations to cloud occurrences than Chlorophyll‐a or Particulate Organic Carbon concentrations Higher nanophytoplankon abundance is positively linked to warm‐liquid cloud frequency of occurrence in spring in most regions of 40°S–60°S Higher nanophytoplankton abundance is linked to a decrease in the ice‐containing cloud frequency of occurrence in most regions

Aerosol mass and the absorbing fraction are important variables, needed to constrain the role of atmospheric particles in the Earth radiation budget, both directly and indirectly through CCN activation. In particular, their monitoring in remote areas and mountain sites is essential for determining source regions, elucidating the mechanisms of long range transport of anthropogenic pollutants, and validating regional and global models. Since March 2006, aerosol mass and black carbon concentration have been monitored at the Nepal Climate Observatory-Pyramid, a permanent high-altitude research station located in the Khumbu valley at 5079 m a.s.l. below Mt. Everest. The first two-year averages of PM1 and PM1−10 mass were 1.94 μg m−3 and 1.88 μg m−3, with standard deviations of 3.90 μg m−3 and 4.45 μg m−3, respectively, while the black carbon concentration average is 160.5 ng m−3, with a standard deviation of 296.1 ng m−3. Both aerosol mass and black carbon show well defined annual cycles, with a maximum during the pre-monsoon season and a minimum during the monsoon. They also display a typical diurnal cycle during all the seasons, with the lowest particle concentration recorded during the night, and a considerable increase during the afternoon, revealing the major role played by thermal winds in influencing the behaviour of atmospheric compounds over the high Himalayas. The aerosol concentration is subject to high variability: in fact, as well as frequent \"background conditions\" (55% of the time) when BC concentrations are mainly below 100 ng m−3, concentrations up to 5 μg m−3 are reached during some episodes (a few days every year) in the pre-monsoon seasons. The variability of PM and BC is the result of both short-term changes due to thermal wind development in the valley, and long-range transport/synoptic circulation. At NCO-P, higher concentrations of PM1 and BC are mostly associated with regional circulation and westerly air masses from the Middle East, while the strongest contributions of mineral dust arrive from the Middle East and regional circulation, with a special contribution from North Africa and South-West Arabian Peninsula in post-monsoon and winter season.

Aerosols of biogenic and anthropogenic origin affect the total radiative forcing of global climate. Poor knowledge of the pre-industrial aerosol concentration and composition, in particular of particles formed directly in the atmosphere from gaseous precursors, constitutes a large uncertainty in the anthropogenic radiative forcing. Investigations of new particle formation at pre-industrial-like conditions can contribute to the reduction of this uncertainty. Here we present observations taken at the remote Nepal Climate Observatory Pyramid station at 5,079 m above sea level, a few kilometres from the summit of Everest. We show that up-valley winds funnel gaseous aerosol precursors to higher altitudes. During this transport, these are oxidized into compounds of very low volatility, which rapidly form a large number of aerosol particles. These are then transported into the free troposphere, which suggests that the whole Himalayan region may act as an ‘aerosol factory’ and contribute substantially to the free tropospheric aerosol population. Aerosol production in this region occurs mainly via organic precursors of biogenic origin with little evidence of the involvement of anthropogenic pollutants. This process is therefore likely to be essentially unchanged since the pre-industrial period, and may have been one of the major sources that contributes to the upper tropospheric aerosol population during that time. Newly formed biogenic particles in the Himalaya increase free-tropospheric background aerosol concentration by a factor of up to two.

This paper provides a detailed description of the atmospheric conditions characterizing the high Himalayas, thanks to continuous observations begun in March 2006 at the Nepal Climate Observatory-Pyramid (NCO-P) located at 5079 m a.s.l. on the southern foothills of Mt. Everest, in the framework of ABC-UNEP and SHARE-Ev-K2-CNR projects. The work presents a characterization of meteorological conditions and air-mass circulation at NCO-P during the first two years of activity. The mean values of atmospheric pressure, temperature and wind speed recorded at the site were: 551 hPa, −3.0 °C, 4.7 m s−1, respectively. The highest seasonal values of temperature (1.7 °C) and relative humidity (94%) were registered during the monsoon season, which was also characterized by thick clouds, present in about 80% of the afternoon hours, and by a frequency of cloud-free sky of less than 10%. The lowest temperature and relative humidity seasonal values were registered during winter, −6.3 °C and 22%, respectively, the season being characterised by mainly cloud-free sky conditions and rare thick clouds. The summer monsoon influenced rain precipitation (seasonal mean: 237 mm), while wind was dominated by flows from the bottom of the valley (S–SW) and upper mountain (N–NE). The atmospheric composition at NCO-P has been studied thanks to measurements of black carbon (BC), aerosol scattering coefficient, PM1, coarse particles and ozone. The annual behaviour of the measured parameters shows the highest seasonal values during the pre-monsoon (BC: 316.9 ng m−3, PM1: 3.9 μg m−3, scattering coefficient: 11.9 Mm−1, coarse particles: 0.37 cm−3 and O3: 60.9 ppbv), while the lowest concentrations occurred during the monsoon (BC: 49.6 ng m−3, PM1: 0.6 μg m−3, scattering coefficient: 2.2 Mm−1, and O3: 38.9 ppbv) and, for coarse particles, during the post-monsoon (0.07 cm−3. At NCO-P, the synoptic-scale circulation regimes present three principal contributions: Westerly, South-Westerly and Regional, as shown by the analysis of in-situ meteorological parameters and 5-day LAGRANTO back-trajectories. The influence of the brown cloud (AOD>0.4) extending over Indo–Gangetic Plains up to the Himalayan foothills has been evaluated by analysing the in-situ concentrations of the ABC constituents. This analysis revealed that brown cloud hot spots mainly influence the South Himalayas during the pre-monsoon, in the presence of very high levels of atmospheric compounds (BC: 1974.1 ng m−3, PM1: 23.5 μg m−3, scattering coefficient: 57.7 Mm−1, coarse particles: 0.64 cm−3, O3: 69.2 ppbv, respectively). During this season 20% of the days were characterised by a strong brown cloud influence during the afternoon, leading to a 5-fold increased in the BC and PM1 values, in comparison with seasonal means. Our investigations provide clear evidence that, especially during the pre-monsoon, the southern side of the high Himalayan valleys represent a \"direct channel\" able to transport brown cloud pollutants up to 5000 m a.s.l., where the pristine atmospheric composition can be strongly influenced.

The formation of new atmospheric particles involves an initial step forming stable clusters less than a nanometre in size (<~1 nm), followed by growth into quasi-stable aerosol particles a few nanometres (~1-10 nm) and larger (>~10 nm). Although at times, the same species can be responsible for both processes, it is thought that more generally each step comprises differing chemical contributors. Here, we present a novel analysis of measurements from a unique multi-station ground-based observing system which reveals new insights into continental-scale patterns associated with new particle formation. Statistical cluster analysis of this unique 2-year multi-station dataset comprising size distribution and chemical composition reveals that across Europe, there are different major seasonal trends depending on geographical location, concomitant with diversity in nucleating species while it seems that the growth phase is dominated by organic aerosol formation. The diversity and seasonality of these events requires an advanced observing system to elucidate the key processes and species driving particle formation, along with detecting continental scale changes in aerosol formation into the future.

Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.

Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May–June and September–October) and 2009 (February–March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.

The effect of ocean acidification and changing water conditions on primary (and secondary) marine aerosol emissions is not well understood on a regional or a global scale. To investigate this effect as well as the indirect effect on aerosol that changing biogeochemical parameters can have, ~ 52 m3 pelagic mesocosms were deployed for several weeks in the Mediterranean Sea during both winter pre-bloom and summer oligotrophic conditions and were subjected to various levels of CO2 to simulate the conditions foreseen in this region for the coming decades. After seawater sampling, primary bubble-bursting aerosol experiments were performed using a plunging water jet system to test both chemical and physical aerosol parameters (10–400 nm). Comparing results obtained during pre-bloom and oligotrophic conditions, we find the same four log-normal modal diameters (18.5 ± 0.6, 37.5 ± 1.4, 91.5 ± 2.0, 260 ± 3.2 nm) describing the aerosol size distribution during both campaigns, yet pre-bloom conditions significantly increased the number fraction of the second (Aitken) mode, with an amplitude correlated to virus-like particles, heterotrophic prokaryotes, TEPs (transparent exopolymeric particles), chlorophyll a and other pigments. Organic fractions determined from kappa closure calculations for the diameter, Dp ~ 50 nm, were much larger during the pre-bloom period (64 %) than during the oligotrophic period (38 %), and the organic fraction decreased as the particle size increased. Combining data from both campaigns together, strong positive correlations were found between the organic fraction of the aerosol and chlorophyll a concentrations, heterotrophic and autotrophic bacteria abundance, and dissolved organic carbon (DOC) concentrations. As a consequence of the changes in the organic fraction and the size distributions between pre-bloom and oligotrophic periods, we find that the ratio of cloud condensation nuclei (CCN) to condensation nuclei (CN) slightly decreased during the pre-bloom period. The enrichment of the seawater samples with microlayer samples did not have any effect on the size distribution, organic content or the CCN activity of the generated primary aerosol. Partial pressure of CO2, pCO2, perturbations had little effect on the physical or chemical parameters of the aerosol emissions, with larger effects observed due to the differences between a pre-bloom and oligotrophic environment.