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- 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
- ItemAerosol number to volume ratios in Southwest Portugal during ACE-2(Milton Park : Taylor & Francis, 2017) Dusek, Ulrike; Covert, David S.; Wiedensohler, Alfred; Neusúss, Christian; Weise, DianaPast studies have indicated that long-term averages of the aerosol number to volume ratios (defined as the number of particles larger than a certain diameter divided by the particle volume over some range less than 1 μm) show little variability over the Atlantic. This work presents number to volume ratios (R) measured during the ACE-2 experiment on the land-based Sagres field site located in Southwest Portugal. The values of R measured in Sagres compare reasonably well with previous measurements over the Atlantic. The main emphasis of this work is therefore to investigate more closely possible reasons for the observed stability of the number to volume ratio. Aerosol number size distributions measured in Sagres are parametrized by the sum of two log-normal distributions fitted to the accumulation and to the Aitken mode. The main factor that limits the variability of R is that the parameters of these log-normal distributions are not always independent but show some covariance. In polluted air mass types correlations between parameters of the Aitken and accumulation mode are mostly responsible for stabilizing R. In marine air mass types the variability of R is reduced by an inverse relationship between the accumulation-mode mean diameter and standard deviation, consistent with condensational processes and cloud processing working on the aerosol. However, despite this reduction, the variability of R in marine air mass types is still considerable and R is linearly dependent on the number concentration of particles larger than 90 nm. This partly due to a mil of Aitken-mode particles extending to sizes larger than 90 nm.
- ItemCloud 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, WillIn 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.