Hygroscopic properties of aerosol particles in the northeastern Atlantic during ACE-2

Measurements 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<RH<95%, and for wind speeds for which the local sea-salt production is small (<ca. 8 m s-1)

Chemical speciation of aerosol samples by ion beam thermography

Ion beam thermography (IBT) is a technique for the determination of chemical compounds. The IBT setup combines the multielemental ion beam techniques PIXE, PESA, pNRA and cPESA with thermography. During thermography the temperature is gradually increased up to the order of 600 °C, causing vaporisation of chemical compounds at specific temperatures. The combination of methods display low detection limits over practically the whole periodic table, i.e. PIXE: Z > 13, PESA: C, N, O, pNRA: Li, Be, B, F, Na, Mg, cPESA: H. The analysis is undertaken with an external beam. The thermographic treatment results in a thermogram for each element i.e. the concentration as a function of the temperature of the sample. The chemical compounds are identified by the vaporisation temperature and the stoichiometric relations between the elements vaporised at that temperature. This work deals with technical improvements of the setup and evaluates the dependence on the rate of temperature increase of the vaporisation temperature of chemical compounds. An atmospheric aerosol sample was analysed to demonstrate the capabilities of this combination of IBA methods in atmospheric aerosol research. All major and several minor elements of the sample could be determined, the major inorganic compounds could be speciated and the carbonaceous constituents could be classified according to volatility

Validation of very high cloud droplet number concentrations in air masses transported thousands of kilometres over the ocean

The microstructure of orographic clouds related to the aerosol present was studied during the second Aerosol Characterisation Experiment (ACE-2). Very high cloud droplet number concentrations (almost 3000 cm -3 ) were observed. These high concentrations occurred when clouds formed on a hill slope at Tenerife in polluted air masses originating in Europe that had transported the order of 1000 km over the Atlantic Ocean. The validity of the measured droplet number concentrations was investigated by comparing with measurements of the aerosol upstream of the cloud and cloud interstitial aerosol. Guided by distributions of the ratios between the measurements, three criteria of typically 30% in maximum deviation were applied to the measurements to test their validity. Agreement was found for 88% of the cases. The validated data set spans droplet number concentrations of 150-3000 cm -3 . The updraught velocity during the cloud formation was estimated to 2.2 m s -1 by model calculations, which is typical of cumuliform clouds. The results of the present study are discussed in relation to cloud droplet number concentrations previously reported in the literature. The importance of promoting the mechanistic understanding of the aerosol/cloud interaction and the use of validation procedures of cloud microphysical parameters is stressed in relation to the assessment of the indirect climatic effect of aerosols

Validation of very high cloud droplet number concentrations in air masses transported thousands of kilometres over the ocean

The microstructure of orographic clouds related to the aerosol present was studied during the second Aerosol Characterisation Experiment (ACE-2). Very high cloud droplet number concentrations (almost 3000 cm -3 ) were observed. These high concentrations occurred when clouds formed on a hill slope at Tenerife in polluted air masses originating in Europe that had transported the order of 1000 km over the Atlantic Ocean. The validity of the measured droplet number concentrations was investigated by comparing with measurements of the aerosol upstream of the cloud and cloud interstitial aerosol. Guided by distributions of the ratios between the measurements, three criteria of typically 30% in maximum deviation were applied to the measurements to test their validity. Agreement was found for 88% of the cases. The validated data set spans droplet number concentrations of 150-3000 cm -3 . The updraught velocity during the cloud formation was estimated to 2.2 m s -1 by model calculations, which is typical of cumuliform clouds. The results of the present study are discussed in relation to cloud droplet number concentrations previously reported in the literature. The importance of promoting the mechanistic understanding of the aerosol/cloud interaction and the use of validation procedures of cloud microphysical parameters is stressed in relation to the assessment of the indirect climatic effect of aerosols

Source identification during the Great Dun Fell Cloud Experiment 1993

A characterisation of the sources influencing the site for the final field campaign of the EUROTRAC subproject GCE (Ground-based Cloud Experiment) at Great Dun Fell, Cumbria, Great Britain in April-May 1993 is presented. The sources were characterised mainly by means of aerosol filter and cascade impactor data, single particle analysis, gas data, data on aromatic organic compounds, cloud water ionic composition, measurements of aerosol size distributions and hygroscopic properties and various meteorological information. Receptor models applied on the aerosol filter and impactor data sets separately revealed two major source types being a marine sea spray source and a long-range transported anthropogenic pollution source. The results of the receptor models were largely consistent with the other observations used in the source identification. Periods of considerable anthropogenic pollution as well as almost pure marine air masses were clearly identified during the course of the experiment