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- ItemAerosol 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, AlfredThe 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.
- ItemA comparison of aerosol chemical and optical properties from the 1st and 2nd Aerosol Characterization Experiments(Milton Park : Taylor & Francis, 2016) Quinn, P.K.; Bates, T.S.; Coffman, D.J.; Coffman, Derek J.; Miller, T.L.; Johnson, J.E.; Covert, D.S.; Putaud, J.- P.; Neusüß, C.; Novakov, T.Shipboard measurements of aerosol chemical composition and optical properties were made during both ACE-1 and ACE-2. ACE-1 focused on remote marine aerosol minimally perturbed by continental sources. ACE-2 studied the outflow of European aerosol into the NE Atlantic atmosphere. A variety of air masses were sampled during ACE-2 including Atlantic, polar, Iberian Peninsula, Mediterranean, and Western European. Reported here are mass size distributions of non-sea salt (nss) sulfate, sea salt, and methanesulfonate and submicron and supermicron concentrations of black and organic carbon. Optical parameters include submicron and supermicron aerosol scattering and backscattering coefficients at 550 nm, the absorption coefficient at 550±20 nm, the Ångström exponent for the 550 and 700 nm wavelength pair, and single scattering albedo at 550 nm. All data are reported at the measurement relative humidity of 55%. Measured concentrations of nss sulfate aerosol indicate that, relative to ACE-1, ACE-2 aerosol during both marine and continental flow was impacted by continental sources. Thus, while sea salt controlled the aerosol chemical composition and optical properties of both the submicron and supermicron aerosol during ACE-1, it played a relatively smaller role in ACE-2. This is confirmed by the larger average Ångström exponent for ACE-2 continental aerosol of 1.2±0.26 compared to the ACE-1 average of -0.03±0.38. The depletion of chloride from sea salt aerosol in ACE-2 continental air masses averaged 55±25% over all particle sizes. This compares to the ACE-2 marine average of 4.8±18% and indicates the enhanced interaction of anthropogenic acids with sea salt as continental air masses are transported into the marine atmosphere. Single scattering albedos averaged 0.95±0.03 for ACE-2 continental air masses. Averages for ACE-2 and ACE-1 marine air masses were 0.98±0.01 and 0.99±0.01, respectively.
- ItemHygroscopic properties of aerosol particles in the northeastern Atlantic during ACE-2(Milton Park : Taylor & Francis, 2016) Swietlicki, Erik; Zhou, Jingchuan; Covert, David S.; Hämeri, Kaarle; Busch, Bernhard; Väkeva, Minna; Dusek, Ulrike; Berg, Olle H.; Wiedensohler, Alfred; Aalto, Pasi; Mäkelä, Jyrki; Martinsson, Bengt G.; Papaspiropoulos, Giorgos; Mentes, Besim; Frank, Göran; Stratmann, FrankMeasurements of the hygroscopic properties of sub-micrometer atmospheric aerosol particles were performed with hygroscopic tandem differential mobility analysers (H-TDMA) at 5 sites in the subtropical north-eastern Atlantic during the second Aerosol Characterization Experiment (ACE-2) from 16 June to 25 July 1997. Four of the sites were in the marine boundary layer and one was, at least occasionally, in the lower free troposphere. The hygroscopic diameter growth factors of individual aerosol particles in the dry particle diameter range 10−440 nm were generally measured for changes in relative humidity (RH) from <10% to 90%. In the marine boundary layer, growth factors at 90% RH were dependent on location, air mass type and particle size. The data was dominated by a unimodal growth distribution of more-hygroscopic particles, although a bimodal growth distribution including less-hygroscopic particles was observed at times, most often in the more polluted air masses. In clean marine air masses the more-hygroscopic growth factors ranged from about 1.6 to 1.8 with a consistent increase in growth factor with increasing particle size. There was also a tendency toward higher growth factors as sodium to sulphate molar ratio increased with increasing sea-salt contribution at higher wind speeds. During outbreaks of European pollution in the ACE-2 region, the growth factors of the largest particles were reduced, but only slightly. Growth factors at all sizes in both clean and polluted air masses were markedly lower at the Sagres, Portugal site due to more proximate continental influences. The frequency of occurrence of less-hygroscopic particles with a growth factor of ca. 1.15 was greatest during polluted conditions at Sagres. The free tropospheric 50 nm particles were predominately less-hygroscopic, with an intermediate growth factor of 1.4, but more-hygroscopic particles with growth factors of about 1.6 were also frequent. While these particles probably originate from within the marine boundary layer, the less-hygroscopic particles are probably more characteristic of lower free tropospheric air masses. For those occasions when measurements were made at 90% and an intermediate 60% or 70% RH, the growth factor G(RH) of the more-hygroscopic particles could be modelled empirically by a power law expression. For the ubiquitous more-hygroscopic particles, the expressions G(RH)=(1-RH/100)-0.210 for 50 nm Aitken mode particles and G(RH)=(1-RH/100)-0.233 for 166 nm accumulation mode particles are recommended for clean marine air masses in the north-eastern Atlantic within the range 0
- ItemSize-segregated chemical, gravimetric and number distribution-derived mass closure of the aerosol in Sagres, Portugal during ACE-2(Milton Park : Taylor & Francis, 2016) Neusüß, C.; Weise, D.; Birmili, W.; Wex, H.; Wiedensohler, A.; Covert, D.S.During the ACE-2 field campaign in the summer of 1997 an intensive, ground-based physical and chemical characterisation of the clean marine and continentally polluted aerosol was performed at Sagres, Portugal. Number size distributions of the dry aerosol in the size range 3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis. Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate the number size distribution at a relative humidity of 60%. A size segregated 3-way mass closure study was performed in this investigation for the first time. Mass size distributions at 60% RH derived from number size distribution measurements and impactors samples (weighing and chemical analysis) are compared. A good agreement was found for the comparison of total gravimetrically-determined mass with both number distribution-derived (slope=1.23/1.09; R2>0.97; depending on the parameters humidity growth and density) and chemical mass concentration (slope=1.02; R2=0.79) for particles smaller than 3 mm in diameter. Except for the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small deviations (R2=0.76–0.98) for the different size fractions were found. Since uncertainties in each of the 3 methods are about 20% the observed differences in the size-segregated mass fractions can be explained by the measurement uncertainties. However, the number distributionderived mass is mostly higher than the chemically and gravimetrically determined mass, which can be explained by sampling losses of the impactor, but as well with measurement uncertainties as, e.g., the sizing of the DMPS/APS.