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)

Studies of Tropospheric and Stratospheric Aerosol using Ion Beam Analysis

Atmospheric aerosol particles are believed to have an impact on the radiative forcing of the earth's surface. The predicted results indicate a net cooling effect on the global climate, however there are few studies available to substantiate this and experimental data are needed. This work deals with the collection and the analysis of aerosol particles in various environments, specifically in the upper tropospheric and lower stratospheric region (the tropopause). As a part of the joint European CARIBIC project, aerosols have been sampled systematically during a two year period from a commercial aircraft during intercontinental flights. The main flight route has been from Germany to Sri Lanka/Maldives. 31 flights have been investigated regarding elemental composition with particle-induced X-ray emission (PIXE). From each flight, both total samples covering the full distance and time resolved samples (2.5 hours time resolution), have been collected. The sampling methodology developed for the special experimental environment at these altitudes is presented in paper I and the first results from this large-scale systematic study are presented in papers II and III. PIXE is multi-elemental and several elements have been detected (e.g. S, K, Fe, Ca, Ti, As, Br) and concentrations of these are presented. Sulphur is the main element of interest and its expected domination is assessed, being a factor of 50 greater in concentration compared to potassium. Seasonal trends have been obtained for sulphur, potassium and iron. The sulphur concentration is also investigated regarding latitude and a clear dependency is found, with a factor of 4 increase from 5 to 50 degrees north in latitude. The stratospheric influence is estimated and found to be significant. The chemical speciation tool Ion Beam Thermography (IBT), combining four elemental ion beam analysis techniques (PIXE, PESA, cPESA and pNRA) with thermography, has been characterised with respect to a number of parameters in paper IV. The chemical compound system sulfuric acid - ammonium sulphate in aerosol samples has been investigated in detail in paper V and the ability of IBT to distinguish the different chemical states of these important constituents of the atmospheric aerosol is assessed

Number and sulfur derived 3-parameter aerosol size distributions in the tropopause region from CARIBIC flights between Germany and the Indic

Aerosol number concentrations in three size ranges (d(p) > 4, d(p) > 12, 18 less than or equal to, dp less than or equal to, 135 nm) and sulfur mass from impactor samples were collected over a total of about 120 sampling hours on 18 long-range commercial flights between the northern mid-latitudes and the equatorial region covering an altitude range between 8.8 and 11.2 km. The data were evaluated with a new random search algorithm to derive monomodal lognormal particle size distributions. Through tests of the algorithm using synthetic data and size distributions from mountain stations the retrieval capabilities of the fitting algorithm are established. The fitting of aerosol data yields three parameters of the submicrometer size distribution. Their latitudinal trends indicate the influence of tropical and mid-latitudinal source regions on the tropopause aerosol. Total particle numbers show maxima near tropical biomass burning, and over the European regions. Geometric mean diameters decrease north of 35degreesN while the width of the distribution increases, indicating a move towards more frequent recent nucleation events or more frequent bimodal size distributions. (C) 2002 Elsevier Science Ltd. All rights reserved

Fine mode particulate sulphur in the tropopause region measured from intercontinental flights (CARIBIC)

Here the first systematic study of the concentration of particulate sulphur in the upper troposphere and lower stratosphere is presented. The measurements were undertaken in the CARIBIC programme during intercontinental flights from a commercial aircraft, which was equipped with an aerosol inlet and a research payload in the cargo bay. Aerosol samples were collected and analysed for elemental composition. The data set comprises 21 flights between Germany and Male/Colombo in the Indian Ocean. The average fine mode, particulate sulphur concentration was 14 ng/m3 STP, which is low compared to remote areas at the Earth's surface. A pronounced dependence with latitude with elevated concentrations occurring within the densely industrialised northern hemispheric mid latitudes was observed, thus suggesting anthropogenic influence on the climate from sulphate particles in the tropopause region

Aerosol elemental concentrations in the tropopause region from intercontinental flights with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform

This study with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform investigates the aerosol elemental concentrations at 9-11 km altitude in the northern hemisphere. Measurements from 31 intercontinental flights over a 2-year period between Germany and Sri Lanka/Maldives in the Indian Ocean are presented. Aerosol samples were collected with an impaction technique and were analyzed for the concentration of 18 elements using particle-induced X-ray emission (PIXE). Additional measurements of particle number concentrations, ozone and carbon monoxide concentrations, and meteorological modeling were included in the interpretation of the aerosol elemental concentrations. Particulate sulphur was found to be by far the most abundant element. Its upper tropospheric concentration increased, on average, by a factor of 2 from the tropics to midlatitudes, with another factor 2 higher concentrations in the lowermost stratosphere over midlatitudes. Correlation patterns and source profiles suggest contributions from crustal sources and biomass burning, but not from meteor ablation. Coinciding latitudinal gradients in particulate sulphur concentrations and emissions suggest that fossil fuel combustion is an important source of the aerosol in the upper troposphere and lowermost stratosphere. The measurements indicate aerosol transport along isentropic surfaces across the tropopause into the lowermost stratosphere. As a result of the prolonged residence time, ageing via oxidation of sulphur dioxide in the lowermost stratosphere was found to be a likely high-altitude, strong source that, along with downward transport of stratospheric air, could explain the vertical gradient of particulate sulphur mass concentration around the extratropical tropopause

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

Hygroscopic properties of aerosol particles in the north-eastern 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)