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    An overview of the Lagrangian experiments undertaken during the North Atlantic regional Aerosol Characterisation Experiment (ACE-2)
    (Milton Park : Taylor & Francis, 2016) Johnson, Doug W.; Osborne, Simon; Wood, Robert; Suhre, Karsten; Johnson, Randy; Businger, Steven; Quinn, Patricia K.; Wiedensohler, Alfred; Durkee, Philip A.; Russell, Lynn M.; Andreae, Meinrat O.; O’Dowd, Colin; Noone, Kevin J.; Bandy, Brian; Rudolph, J.; Rapsomanikis, Spyros
    One of the primary aims of the North Atlantic regional Aerosol Characterisation Experiment (ACE-2) was to quantify the physical and chemical processes affecting the evolution of the major aerosol types over the North Atlantic. The best, practical way of doing this is in a Lagrangian framework where a parcel of air is sampled over several tens of hours and its physical and chemical properties are intensively measured. During the intensive observational phase of ACE-2, between 15 June 1997 and 24 July 1997, 3 cloudy Lagrangian experiments and 3 cloud-free, Lagrangian experiments were undertaken between the south west tip of the Iberian Peninsula and the Canary Islands. This paper gives an overview of the aims and logistics of all of the Lagrangian experiments and compares and contrasts them to provide a framework for the more focused Lagrangian papers in this issue and future process modelling studies and parametrisation development. The characteristics of the cloudy Lagrangian experiments were remarkably different, enabling a wide range of different physical and chemical processes to be studied. In the 1st Lagrangian, a clean maritime air mass was sampled in which salt particle production, due to increased wind speed, dominated the change in the accumulation mode concentrations. In the 2nd Lagrangian, extensive cloud cover resulted in cloud processing of the aerosol in a polluted air mass, and entrainment of air from the free troposphere influenced the overall decrease in aerosol concentrations in the marine boundary layer (MBL). Very little change in aerosol characteristics was measured in the 3rd Lagrangian, where the pollution in the MBL was continually being topped up by entraining air from a residual continental boundary layer (CBL) above. From the analysis of all the Lagrangian experiments, it has been possible to formulate, and present here, a generalised description of a European continental outbreak of pollution over the sub-tropical North Atlantic.
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    Variability of sub-micrometer particle number size distributions and concentrations in the Western Mediterranean regional background
    (Milton Park : Taylor & Francis, 2013) Cusack, Michael; Pérez, NoemÍ; Pey, Jorge; Wiedensohler, Alfred; Alastuey, Andrés
    This study focuses on the daily and seasonal variability of particle number size distributions and concentrations, performed at the Montseny (MSY) regional background station in the western Mediterranean from October 2010 to June 2011. Particle number concentrations at MSY were shown to be within range of various other sites across Europe reported in literature, but the seasonality of the particle number size distributions revealed significant differences. The Aitken mode is the dominant particle mode at MSY, with arithmetic mean concentrations of 1698 cm3, followed by the accumulation mode (877 cm3) and the nucleation mode (246 cm3). Concentrations showed a strong seasonal variability with large increases in particle number concentrations observed from the colder to warmer months. The modality of median size distributions was typically bimodal, except under polluted conditions when the size distribution was unimodal. During the colder months, the daily variation of particle number size distributions are strongly influenced by a diurnal breeze system, whereby the Aitken and accumulation modes vary similarly to PM1 and BC mass concentrations, with nocturnal minima and sharp day-time increases owing to the development of a diurnal mountain breeze. Under clean air conditions, high levels of nucleation and lower Aitken mode concentrations were measured, highlighting the importance of new particle formation as a source of particles in the absence of a significant condensation sink. During the warmer months, nucleation mode concentrations were observed to be relatively elevated both under polluted and clean conditions due to increased photochemical reactions, with enhanced subsequent growth owing to elevated concentrations of condensable organic vapours produced from biogenic volatile organic compounds, indicating that nucleation at MSY does not exclusively occur under clean air conditions. Finally, mixing of air masses between polluted and non-polluted boundary layer air, and brief changes in the air mass being sampled gave rise to unusual particle number size distributions, with specific cases of such behaviour discussed at length.
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    In situ aerosol characterization at Cape Verde, Part 2: Parametrization of relative humidity- and wavelength-dependent aerosol optical properties
    (Milton Park : Taylor & Francis, 2017) Schladitz, Alexander; Müller, Thomas; Nordmann, Stephan; Tesche, Matthias; Silke Groß, Silke Groß; Freudenthaler, Volker; Gasteiger, Josef; Wiedensohler, Alfred
    An observation-based numerical study of humidity-dependent aerosol optical properties of mixed marine and Saharan mineral dust aerosol is presented. An aerosol model was developed based on measured optical and microphysical properties to describe the marine and Saharan dust aerosol at Cape Verde. A wavelength-dependent optical equivalent imaginary part of the refractive index and a scattering non-sphericity factor for Saharan dustwere derived. Simulations of humidity effects on optical properties by the aerosol model were validated with relative measurements of the extinction coefficient at ambient conditions. Parametrizations were derived to describe the humidity dependence of the extinction, scattering, and absorption coefficients as well as the asymmetry parameter and single scattering albedo. For wavelengths (300–950 nm) and dry dust volume fractions (0–1), aerosol optical properties as a function of relative humidity (RH = 0–90%) can be calculated from tabulated parameters. For instance, at a wavelength of 550 nm, a volume fraction of 0.5 of dust on the total particle volume (dry conditions) and a RH of 90%, the enhancements for the scattering, extinction and absorption coefficients are 2.55, 2.46 and 1.04, respectively, while the enhancements for the asymmetry parameter and single scattering albedo are 1.11 and 1.04.
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    Occurrence of an ultrafine particle mode less than 20 nm in diameter in the marine boundary layer during Arctic summer and autumn
    (Milton Park : Taylor & Francis, 2017) Wiedensohler, Alfred; Covert, David S.; Swietlicki, Erik; Aalto, Pasi; Heintzenberg, Jost; Leck, Caroline
    The International Arctic Ocean Expedition 1991 (IAOE-91) provided a platform to study the occurrence and size distributions of ultrafine particles in the marine boundary layer (MBL) during Arctic summer and autumn. Measurements of both aerosol physics, and gas/particulate chemistry were taken aboard the Swedish icebreaker Oden. Three separate submicron aerosol modes were found: an ultrafine mode (Dp < 20 nm), the Aitken mode (20 < Dp < 100 nm), and the accumulation mode (Dp > 100 nm). We evaluated correlations between ultrafine particle number concentrations and mean diameter with the entire measured physical, chemical, and meteorological data set. Multivariate statistical methods were then used to make these comparisons. A principal component (PC) analysis indicated that the observed variation in the data could be explained by the influence from several types of air masses. These were characterised by contributions from the open sea or sources from the surrounding continents and islands. A partial least square (PLS) regression of the ultrafine particle concentration was also used. These results implied that the ultrafine particles were produced above or in upper layers of the MBL and mixed downwards. There were also indications that the open sea acted as a source of the precursors for ultrafine particle production. No anti-correlation was found between the ultrafine and accumulation particle number concentrations, thus indicating that the sources were in separate air masses.
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    Cloud condensation nuclei spectra derived from size distributions and hygroscopic properties of the aerosol in coastal south-west Portugal during ACE-2
    (Milton Park : Taylor & Francis, 2016) Dusek, Ulrike; Covert, David S.; Wiedensohler, Alfred; Neusüss, Christian; Weise, Diana; Cantrell, Will
    In this work we propose and test a method to calculate cloud condensation nuclei (CCN) spectra basedon aerosol number size distributions and hygroscopic growth factors. Sensitivity studies show thatthis method can be used in a wide variety of conditions except when the aerosol consist mainly oforganic compounds. One crucial step in the calculations, estimating soluble ions in an aerosol particlebased on hygroscopic growth factors, is tested in an internal hygroscopic consistency study. The resultsshow that during the second Aerosol Characterization Experiment (ACE-2) the number concentrationof inorganic ions analyzed in impactor samples could be reproduced from measured growth factorswithin the measurement uncertainties at the measurement site in Sagres, Portugal. CCN spectra were calculated based on data from the ACE-2 field experiment at the Sagres site.The calculations overestimate measured CCN spectra on average by approximately 30%, which iscomparable to the uncertainties in measurements and calculations at supersaturations below 0.5%. Thecalculated CCN spectra were averaged over time periods when Sagres received clean air masses and airmasses influenced by aged and recent pollution. Pollution outbreaks enhance the CCN concentrationsat supersaturations near 0.2% by a factor of 3 (aged pollution) to 5 (recent pollution) compared to theclean marine background concentrations. In polluted air masses, the shape of the CCN spectra changes.The clean spectra can be approximated by a power function, whereas the polluted spectra are betterapproximated by an error function.
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    Study of the relative humidity dependence of aerosol light-scattering in southern Spain
    (Milton Park : Taylor & Francis, 2014) Titos, Gloria; Lyamani, Hassan; Cazorla, Alberto; Sorribas, Mar; Foyo-Moreno, Inmaculada; Wiedensohler, Alfred; Alados-Arboledas, Lucas
    This investigation focuses on the characterisation of the aerosol particle hygroscopicity. Aerosol particle optical properties were measured at Granada, Spain, during winter and spring seasons in 2013. Measured optical properties included particle light-absorption coefficient (σap) and particle light-scattering coefficient (σsp) at dry conditions and at relative humidity (RH) of 85±10%. The scattering enhancement factor, f(RH=85%), had a mean value of 1.5±0.2 and 1.6±0.3 for winter and spring campaigns, respectively. Cases of high scattering enhancement were more frequent during the spring campaign with 27% of the f(RH=85%) values above 1.8, while during the winter campaign only 8% of the data were above 1.8. A Saharan dust event (SDE), which occurred during the spring campaign, was characterised by a predominance of large particles with low hygroscopicity. For the day when the SDE was more intense, a mean daily value of f(RH=85%)=1.3±0.2 was calculated. f(RH=85%) diurnal cycle showed two minima during the morning and afternoon traffic rush hours due to the increase in non-hygroscopic particles such as black carbon and road dust. This was confirmed by small values of the single-scattering albedo and the scattering Ångstrom exponent. A significant correlation between f(RH=85%) and the fraction of particulate organic matter and sulphate was obtained. Finally, the impact of ambient RH in the aerosol radiative forcing was found to be very small due to the low ambient RH. For high RH values, the hygroscopic effect should be taken into account since the aerosol forcing efficiency changed from −13 W/m2 at dry conditions to −17 W/m2 at RH=85%.
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    A simple non-linear analytical relationship between aerosol accumulation number and sub-micron volume, explaining their observed ratio in the clean and polluted marine boundary layer
    (Milton Park : Taylor & Francis, 2016) Van Dingenen, Rita; Virkkula, Aki O.; Raes, Frank; Bates, Timothy S.; Wiedensohler, Alfred
    We propose an analytical expression for the relation between aerosol accumulation number and sub-micron volume over the marine boundary layer (MBL), based on a simple balance equation. By providing appropriate source and sink terms which account for entrainment, coagulation, in-cloud scavenging and condensational growth, the model is able to reproduce the observed ratio between MBL particles larger than 80 nm diameter (as a proxy for accumulation mode number) and submicron aerosol volume, from freshly polluted to background conditions. Entrainment and coagulation are essential in predicting the observed ratio. Budget and lifetime calculations show that, due to relatively low source rates of oceanic non-sea-salt-sulfate and sea-salt, the anthropogenic signature in aerosol volume remains significant even after 8 days of MBL transport.
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    Aerosol physical properties and processes in the lower marine boundary layer: A comparison of shipboard sub-micron data from ACE-1 and ACE-2
    (Milton Park : Taylor & Francis, 2016) Bates, Timothy S.; Quinn, Patricia K.; Covert, David S.; Coffman, Derek J.; Johnson, James E.; Wiedensohler, Alfred
    The goals of the IGAC Aerosol Characterization Experiments (ACE) are to determine and understand the properties and controlling processes of the aerosol in a globally representative range of natural and anthropogenically perturbed environments. ACE-1 was conducted in the remote marine atmosphere south of Australia while ACE-2 was conducted in the anthropogenically modified atmosphere of the Eastern North Atlantic. In-situ shipboard measurements from the RV Discoverer(ACE-1) and the RV Professor Vodyanitskiy(ACE-2), combined with calculated back trajectories can be used to define the physical properties of the sub-micron aerosol in marine boundary layer (MBL) air masses from the remote Southern Ocean, Western Europe, the Iberian coast, the Mediterranean and the background Atlantic Ocean. The differences in these aerosol properties, combined with dimethylsulfide, sulfur dioxide and meteorological measurements provide a means to assess processes that affect the aerosol distribution. The background sub-micron aerosol measured over the Atlantic Ocean during ACE-2 was more abundant (number and volume) and appeared to be more aged than that measured over the Southern Ocean during ACE-1. Based on seawater DMS measurements and wind speed, the oceanic source of non-sea-salt sulfur and sea-salt to the background marine atmosphere during ACE-1 and ACE-2 was similar. However, the synoptic meteorological pattern was quite different during ACE-1 and ACE-2. The frequent frontal passages during ACE-1 resulted in the mixing of nucleation mode particles into the marine boundary layer from the free troposphere and relatively short aerosol residence times. In the more stable meteorological setting of ACE-2, a significant nucleation mode aerosol was observed in the MBL only for a half day period associated with a weak frontal system. As a result of the longer MBL aerosol residence times, the average background ACE-2 accumulation mode aerosol had a larger diameter and higher number concentration than during ACE-1. The sub-micron aerosol number size distributions in the air masses that passed over Western Europe, the Mediterranean, and coastal Portugal were distinctly different from each other and the background aerosol. The differences can be attributed to the age of the air mass and the degree of cloud processing.
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    In situ aerosol characterization at Cape Verde, Part 1: Particle number size distributions, hygroscopic growth and state of mixing of the marine and Saharan dust aerosol
    (Milton Park : Taylor & Francis, 2017) Schladitz, Alexander; Müller, Thomas; Nowak, Andreas; Kandler, Konrad; Lieke, Kirsten; Massling, Andreas; Wiedensohler, Alfred
    Particle number size distributions and hygroscopic properties of marine and Saharan dust aerosol were investigated during the SAMUM-2 field study at Cape Verde in winter 2008. Aitken and accumulation mode particles were mainly assigned to the marine aerosol, whereas coarse mode particles were composed of sea-salt and a variable fraction of Saharan mineral dust. A new methodical approach was used to derive hygroscopic growth and state of mixing for a particle size range (volume equivalent) from dpve = 26 nm to 10 μm. For hygroscopic particles with dpve < 100 nm, the median hygroscopicity parameter κ is 0.35. From 100 nm < dpve < 350 nm, κ increases to 0.65. For larger particles, κ at dpve = 350 nm was used. For nearly hydrophobic particles, κ is between 0 and 0.1 for dpve < 250 nm and decreases to 0 for dpve > 250 nm. The mixing state of Saharan dust in terms of the number fraction of nearly hydrophobic particles showed the highest variation and ranges from 0.3 to almost 1. This study was used to perform a successful mass closure at ambient conditions and demonstrates the important role of hygroscopic growth of large sea-salt particles.
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    Characterization of the planetary boundary layer during SAMUM-2 by means of lidar measurements
    (Milton Park : Taylor & Francis, 2017) Groß, Silke; Gasteiger, Josef; Freudenthaler, Volker; Wiegner, Matthias; Geiß, Alexander; Schladitz, Alexander; Toledano, Carlos; Kandler, Konrad; Tesche, Matthias; Ansmann, Albert; Wiedensohler, Alfred
    Measurements with two Raman-depolarization lidars of the Meteorological Institute of the Ludwig-Maximilians- Universit¨at, M¨unchen, Germany, performed during SAMUM-2, were used to characterize the planetary boundary layer (PBL) over Praia, Cape Verde. A novel approach was used to determine the volume fraction of dust υd in the PBL. This approach primarily relies on accurate measurements of the linear depolarization ratio. Comparisons with independent in situ measurements showed the reliability of this approach. Based on our retrievals, two different phases could be distinguished within the measurement period of almost one month. The first (22–31 January 2008) was characterized by high aerosol optical depth (AOD) in the PBL and large υd > 95%. During the second phase, the AOD in the PBL was considerably lower and υd less than ∼40%. These findings were in very good agreement with ground based in situ measurements, when ambient volume fractions are considered that were calculated from the actual measurements of the dry volume fraction. Only in cases when dust was not the dominating aerosol component (second phase), effects due to hygroscopic growth became important.