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The formation and development of orographic clouds was studied in a field experiment comprising several measurement sites at a mountain ridge. The influence of the aerosol population present on the cloud microstructure was studied in relation to the dynamics in the cloud formation. Droplet nucleation scavenging was investigated by the introduction of a non-dimensional particle diameter related to the process, and it was found that the scavenging rose rapidly in a relatively narrow particle size interval. The size dependency of the scavenging could partly be explained by external mixture of the aerosol. The large particles in the cloud interstitial aerosol was found to be of a chemical nature which allows for only a very weak uptake of water, implying that the chemical composition of these particles rather than entrainment of dry air prevented the droplet nucleation. The aerosol particle number concentration was found to strongly influence the cloud microstructure. Droplet number concentrations up to approximately 2000 cm −3 were observed together with a substantially reduced effective droplet diameter. The observed effect of elevated particle number concentrations in orographic clouds was generalised to the climatologically more important stratiform clouds by the use of a cloud model. It was found that the microstructure of stratiform clouds was strongly dependent on the aerosol population present as well on the dynamics in the cloud formation.

The hygroscopic properties of sub-micrometer aerosol particles were studied in connection with a ground-based cloud experiment at Great Dun Fell, in northern England in 1995. Hygroscopic diameter growth factors were measured with a Tandem Differential Mobility Analyser (TDMA) for dry particle diameters between 35 and 265 nm at one of the sites upwind of the orographic cloud. An external mixture consisting of three groups of particles, each with different hygroscopic properties, was observed. These particle groups were denoted less-hygroscopic, more-hygroscopic and sea spray particles and had average diameter growth factors of 1.11–1.15, 1.38–1.69 and 2.08–2.21 respectively when taken from a dry state to a relative humidity of 90%. Average growth factors increased with dry particle size. A bimodal hygroscopic behaviour was observed for 74–87% of the cases depending on particle size. Parallel measurements of dry sub-micrometer particle number size distributions were performed with a Differential Mobility Particle Sizer (DMPS). The inorganic ion aerosol composition was determined by means of ion chromatography analysis of samples collected with Berner-type low pressure cascade impactors at ambient conditions. The number of ions collected on each impactor stage was predicted from the size distribution and hygroscopic growth data by means of a model of hygroscopic behaviour assuming that only the inorganic substances interacted with the ambient water vapour. The predicted ion number concentration was compared with the actual number of all positive and negative ions collected on the various impactor stages. For the impactor stage which collected particles with aerodynamic diameters between 0.17–0.53 μm at ambient relative humidity, and for which all pertinent data was available for the hygroscopic closure study, the predicted ion concentrations agreed with the measured values within the combined measurement and model uncertainties for all cases but one. For this impactor sampling occasion, the predicted ion concentration was significantly higher than the measured. The air mass in which this sample was taken had undergone extensive photochemical activity which had probably produced hygroscopically active material other than inorganic ions, such as organic oxygenated substances.

Cloud condensation nucleus concentration (CCN) was measured directly at a supersaturation of 0.5% with a thermal gradient diffusion cloud chamber at Cape Grim, Tasmania, during the First Aerosol Characterization Experiment (ACE 1) field study in November and December of 1995. Number-size distributions N(Dp) from 3 to 800 nm diameter and the hygroscopic properties of the aerosol in the 30 to 300 nm diameter range (which contains most of the CCN active at 0.5%) were measured concurrently at the same location. This data set provides a basis to compare measured and modeled CCN concentrations. A critical particle diameter that would form cloud droplets at 0.5% supersaturation was derived from the hygroscopic growth data including consideration of the hydration of the size distribution measurement. This empirically derived diameter incorporates the effects of soluble and insoluble mass as well as an effective van't Hoff factor and surface tension as described by Kohler theory for heterogeneous nucleation of cloud droplets. The size distributions were integrated for diameters greater than the critical value and compared to the directly measured CCN concentrations. The modeled CCN concentration was 95 cm−3 during baseline sector periods and 128 cm−3 overall. This was about 20% greater than the directly measured CCN concentration and well correlated (R2 = 0.7) with measured CCN. Two thirds of the CCN at 0.5% supersaturation derive from an accumulation mode (80 nm 200 nm) and the Aitken mode (Dp < 80 nm). The data include air masses from continental, anthropogenic, and biomass burning sources as well as the more dominant marine source.

The present study comprises a large body of physical and chemical mass-related aerosol data which were collected over the industrialized basin of Leipzig, Germany, during the time period 1983 to 1997. For the period 1996/1997 consistent mass size distributions over the range 0.01 to 10 μm (PM10) were determined with a differential mobility analyzer and an aerodynamic particle sizer. The modal size distribution parameters were compared to similar lognormal data from the United States of the 1970s, yielding lower concentrations and coarse particle geometric diameters. In both accumulation and coarse mode, narrower distributions than over the United States were found which may be real or due to instrumental limitations in the 1970s. Within the range of measurement uncertainties and with reasonable assumptions about particle densities, chemical mass closure could be achieved with results of daily PMl0 samples. However, the results of a harmonic analysis of the physical and chemical time series indicated that there may be significant aerosol components which were not covered by our analyses, possibly organic compounds. Since 1990 a significant downward trend in gravimetric mass concentration and since 1993 clear changes in aerosol composition were found which are consistent with similar findings in precipitation samples over eastern Germany.

The droplet activation process and droplet growth was studied during early stages of the formation of orographically-induced clouds. The experimental results were compared with the results obtained with a closed parcel, adiabatic cloud model. Good agreement was in most cases found between model and measurements with respect to cloud droplet number concentration, cloud droplet solute concentration and particle sizes scavenged due to cloud droplet nucleation. The experimental results were mainly obtained with a new instrument, the droplet aerosol analyser (DAA), which allows the determination of ambient sizes of cloud droplets and interstitial aerosol particles directly connected with the size of its dry residue in a two-parameter data acquisition. The resulting three-dimensional data set (ambient size, dry size, number concentration) was utilised to determine several cloud/aerosol properties, whereof some unique.

The 1993 Ground-based Cloud Experiment on Great Dun Fell used a wide range of measurements of trace gases, aerosol particles and cloud droplets at five sites to study their sources and sinks especially those in cloud. These measurements have been interpreted using a variety of models. The conclusions add to our knowledge of air pollution, acidification of the atmosphere and the ground, eutrophication and climate change. The experiment is designed to use the hill cap cloud as a flow-through reactor, and was conducted in varying levels of pollution typical of much of the rural temperate continental northern hemisphere in spring-time.

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.

Synoptic and local meteorological conditions during the Spring 1993 Ground-based Cloud Experiment on Great Dun Fell are described, including cloud microphysics, general pollution levels and sources of air, especially for five case studies selected for detailed analysis. Periods when air was flowing across the hill are identified and the extent to which air mixed into the cloud from above reached the ground is estimated. To aid the interpretation of cloud chemistry and microphysics measurements, the horizontal and vertical extent of the cloud are used to estimate droplet lifetimes and to comment on the influence of complex terrain on peak supersaturation.

The formation and occurrence of new ultrafine aerosol particles were studied in association with an orographic cloud during a field experiment at Great Dun Fell (GDF), Northern England. Three size spectrometers to measure submicrometer aerosol particles were located upwind, on top, and downwind of GDF Summit to investigate changes in the aerosol size distribution. During two night-time cloud periods, ultrafine particles were observed downwind of the hill while no particles were detected upwind of the hill. During one cloud event, there was some evidence of entrainment. In this case, the occurrence of ultrafine particles may have been due to entrainment from aloft or by homogenous nucleation downwind of the hill. During the other cloud event, the formation of an ultrafine particle mode (nucleation mode) occurred probably after the cloud passage. There was no evidence of entrainment during this time period. Multicomponent homogeneous nucleation models were used to simulate the formation of new particle downwind of an orographic cloud. Possible homogeneous nucleation processes for this could be the formation of sulphuric acid or ammonium chloride due to outgassing of hydrochloric acid. It was not possible, however, to simulate formation rates of new particles as observed downwind the hill using a model for the binary or ternary homogeneous nucleation process of ammonia and hydrochloric acid. During the first event with high sulphur dioxide concentrations, the formation of new particle via binary homogeneous nucleation of sulphuric acid and water could be only predicted using a high nighttime hydroxyl radical concentration. No formation of sulphuric acid particle could be simulated during the second event with low sulphur dioxide concentrations.

The size distributions and hygroscopic growth spectra of aerosol particles were measured during the GCE cloud experiment at Great Dun Fell in the Pennine Hills in northern England. Hygroscopic growth is defined as the particle diameter at 90% RH divided by the particle diameter at 10% RH. The fraction of the aerosol particles scavenged by cloud droplets as a function of particle size was also measured. The general aerosol type was a mixture of marine and aged anthropogenic aerosols. The Aitken and accumulation mode numbers (average ± 1 S.D.) were 1543 ± 1078 and 1023 ± 682 cm−3 respectively. The mean diameters were in the range 30–100 nm and 100–330 nm. The hygroscopic growth spectra were bimodal about half the time. The less-hygroscopic particles had average growth factors of 1.06, 1.06, 1.03, 1.03, and 1.03 for particle diameters of 50, 75, 110, 165, and 265 nm, respectively. For the more-hygroscopic particles of the same sizes, the average hygroscopic growth was 1.34, 1.37, 1.43, 1.47, and 1.53. The effects of ageing on the aerosol particle size distribution and on hygroscopic behaviour are discussed. The scavenged fraction of aerosol particles was a strong function of particle diameter. The diameter with 50% scavenging was in the range 90–220 nm. No tail of smaller particles activated to cloud drops was observed. A small tail of larger particles that remained in the interstitial aerosol can be explained by there being a small fraction of less-hygroscopic particles. A weak correlation between the integral dry particle diameter and the diameter with 50% scavenging was seen.

Observations are presented of the aerosol size distribution both upwind and downwind of the Great Dun Fell cap cloud. Simultaneous measurements of the cloud microphysics and cloud chemistry, and of the chemical composition of the aerosol both upwind and downwind of the hill were made along with measurements of sulphur dioxide, hydrogen peroxide and ozone. These observations are used for initialisation of, and for comparison with the predictions of a model of the air flow, cloud microphysics and cloud chemistry of the system. A broad droplet size distribution is often observed near to the hill summit, seemingly produced as a result of a complex supersaturation profile and by mixing between parcels with different ascent trajectories. The model generates several supersaturation peaks as the airstream ascends over the complex terrain, activating increasing numbers of droplets. In conditions where sulphate production in-cloud (due to the oxidation of S(IV) by hydrogen peroxide and ozone) is observed, there is a marked effect on the chemical evolution of the aerosol particles on which the droplets form. When sulphate production occurs, a significant modification of the aerosol size distribution and hygroscopic properties is both predicted and observed. The addition of sulphate mass to those aerosol particles nucleation scavenged by the cloud generally increases the ease with which they are subsequently able to act as cloud condensation nuclei (CCN). Often, this will lead to an increase in the number of CCN available for subsequent cloud formation, although this latter effect is shown to be strongly dependent upon the activation history of the droplets and the concentration of pollutant gases present in the interstitial air. Situations are also identified where cloud processing could lead to a reduction in the capacity of smaller aerosol to act as CCN.

In order to study the relation between the initial aerosol particle spectrum at cloud base and the resulting droplet spectrum in cloud for the “Ground-based Cloud Experiment” field campaign at the Great Dun Fell in 1993 numerical model simulations have been performed. The droplet spectra were calculated from a microphysical model coupled to a dynamic air flow model. The resulting droplet spectra were compared with cloud droplet spectra measured with a forward scattering spectrometer probe. The size distribution and chemical composition of the initial aerosol population were derived from a combination of size distribution and size-segregated chemical measurements below cloud base. From this we concluded that the aerosol particles consisted almost entirely of an inorganic salt. As part of the sensitivity studies two different microphysical models were used, as well as the dynamic flow fields from two different air flow models. As in previous studies we found that the measured droplet spectra were broader and contained larger drops than the modelled spectra. From the sensitivity studies we identified fluctuations in the dynamics as the most likely explanation for these differences.

Diffusion losses and charging efficiency were measured for three types of charge neutralizers commonly used in aerosol research: two with 85Kr and one with 210Po as radiation sources. The diffusion losses were characterized at flows of 0.5 -6 1 min−1 typically used in atmospheric aerosol physics measurements. All of the neutralizers tested exhibited high transmission efficiencies, with losses up to 25% at the smallest tested size of 3 nm, varying with size and flow in general agreement with diffusion loss theory. Charging efficiency was measured for a singly charged, monodisperse aerosol at the same flows and at concentrations of 103-104 particles cm−3. Neither of the 85Kr chargers brought the charge distribution close to equilibrium at 2 1 min−1, except at concentrations ≤ 103 cm−3. The 210Po charger produced the theoretically expected fraction of singly charged particles within the uncertainty of the experiment.

Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal-optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R-2 = 0.67-0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA(2)-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal behaviour and chemical composition of the ATOFMS classes also enabled estimation of the relative contribution of transported emissions of each chemical species and total particle mass in the size range investigated. Only 22% of the total ATOFMS-derived particle mass was apportioned to fresh, local emissions, with 78% apportioned to regional/continental-scale emissions. Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal-optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R-2 = 0.67-0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA(2)-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal behaviour and chemical composition of the ATOFMS classes also enabled estimation of the relative contribution of transported emissions of each chemical species and total particle mass in the size range investigated. Only 22% of the total ATOFMS-derived particle mass was apportioned to fresh, local emissions, with 78% apportioned to regional/continental-scale emissions.

We have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001–2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.

A long term experiment was conducted in a primary forest area in Amazonia, with continuous in-situ measurements of aerosol optical properties between February 2008 and April 2011, comprising, to our knowledge, the longest database ever in the Amazon Basin. Two major classes of aerosol particles, with significantly different optical properties were identified: coarse mode predominant biogenic aerosols in the wet season (January–June), naturally released by the forest metabolism, and fine mode dominated biomass burning aerosols in the dry season (July–December), transported from regional fires. Dry particle median scattering coefficients at the wavelength of 550 nm increased from 6.3 Mm−1 to 22 Mm−1, whereas absorption at 637 nm increased from 0.5 Mm−1 to 2.8 Mm−1 from wet to dry season. Most of the scattering in the dry season was attributed to the predominance of fine mode (PM2) particles (40–80% of PM10 mass), while the enhanced absorption coefficients are attributed to the presence of light absorbing aerosols from biomass burning. As both scattering and absorption increased in the dry season, the single scattering albedo (SSA) did not show a significant seasonal variability, in average 0.86 ± 0.08 at 637 nm for dry aerosols. Measured particle optical properties were used to estimate the aerosol forcing efficiency at the top of the atmosphere. Results indicate that in this primary forest site the radiative balance was dominated by the cloud cover, particularly in the wet season. Due to the high cloud fractions, the aerosol forcing efficiency absolute values were below −3.5 W m−2 in 70% of the wet season days and in 46% of the dry season days. Besides the seasonal variation, the influence of out-of-Basin aerosol sources was observed occasionally. Periods of influence of the Manaus urban plume were detected, characterized by a consistent increase on particle scattering (factor 2.5) and absorption coefficients (factor 5). Episodes of biomass burning and mineral dust particles advected from Africa were observed between January and April, characterized by enhanced concentrations of crustal elements (Al, Si, Ti, Fe) and potassium in the fine mode. During these episodes, median particle absorption coefficients increased by a factor of 2, whereas median SSA values decreased by 7%, in comparison to wet season conditions.

The atmospheric concentration of elemental carbon (EC) in Europe during the six-year period 2005-2010 has been simulated with the EMEP MSC-W model. The model bias compared to EC measurements was less than 20% for most of the examined sites. The model results suggest that fossil fuel combustion is the dominant source of EC in most of Europe but that there are important contributions also from residential wood burning during the cold seasons and, during certain episodes, also from open biomass burning (wildfires and agricultural fires). The modelled contributions from open biomass fires to ground level concentrations of EC were small at the sites included in the present study, EC measurements and modelled EC were also compared to optical measurements of black carbon (BC). The relationships between EC and BC (as given by mass absorption cross section, MAC, values) differed widely between the sites, and the correlation between observed EC and BC is sometimes poor, making it difficult to compare results using the two techniques and limiting the comparability of BC measurements to model EC results. A new bottom-up emission inventory for carbonaceous aerosol from residential wood combustion has been applied. For some countries the new inventory has substantially different EC emissions compared to earlier estimates. For northern Europe the most significant changes are much lower emissions in Norway and higher emissions in neighbouring Sweden and Finland. For Norway and Sweden, comparisons to source-apportionment data from winter campaigns indicate that the new inventory may improve model-calculated EC from wood burning. Finally, three different model setups were tested with variable atmospheric lifetimes of EC in order to evaluate the model sensitivity to the assumptions regarding hygroscopicity and atmospheric ageing of EC. The standard ageing scheme leads to a rapid transformation of the emitted hydrophobic EC to hygroscopic particles, and generates similar results when assuming that all EC is aged at the point of emission. Assuming hydrophobic emissions and no ageing leads to higher EC concentrations. For the more remote sites, the observed EC concentration was in between the modelled EC using standard ageing and the scenario treating EC as hydrophobic. This could indicate too-rapid EC ageing in the model in relatively clean parts of the atmosphere. © Author(s) 2013. CC Attribution 3.0 License.

Atmospheric aerosol particles influence the climate system directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. Apart from black carbon aerosol, aerosols cause a negative radiative forcing at the top of the atmosphere and substantially mitigate the warming caused by greenhouse gases. In the future, tightening of controls on anthropogenic aerosol and precursor vapour emissions to achieve higher air quality may weaken this beneficial effect. Natural aerosols, too, might affect future warming. Here we analyse long-term observations of concentrations and compositions of aerosol particles and their biogenic precursor vapours in continental mid- and high-latitude environments. We use measurements of particle number size distribution together with boundary layer heights derived from reanalysis data to show that the boundary layer burden of cloud condensation nuclei increases exponentially with temperature. Our results confirm a negative feedback mechanism between the continental biosphere, aerosols and climate: aerosol cooling effects are strengthened by rising biogenic organic vapour emissions in response to warming, which in turn enhance condensation on particles and their growth to the size of cloud condensation nuclei. This natural growth mechanism produces roughly 50% of particles at the size of cloud condensation nuclei across Europe. We conclude that biosphere-atmosphere interactions are crucial for aerosol climate effects and can significantly influence the effects of anthropogenic aerosol emission controls, both on climate and air quality. © 2013 Macmillan Publishers Limited. All rights reserved.

International audience; The effect of a post-industrial megacity on local and regional air quality was assessed via a month-long field measurement campaign in the Paris metropolitan area during winter 2010. Here we present source apportionment results from three aerosol mass spectrometers and two aethalome-ters deployed at three measurement stations within the Paris region. Submicron aerosol composition is dominated by the organic fraction (30–36 %) and nitrate (28–29 %), with lower contributions from sulfate (14–16 %), ammonium (12–14 %) and black carbon (7–13 %). Organic source apportionment was performed using positive matrix factorization, resulting in a set of organic factors corresponding both to primary emission sources and secondary production. The dominant primary sources are traffic (11–15 % of organic mass), biomass burning (13–15 %) and cooking (up to 35 % during meal hours). Secondary organic aerosol contributes more than 50 % to the total organic mass and includes a highly oxidized factor from indeterminate and/or diverse sources and a less oxidized factor related to wood burning emissions. Black carbon was apportioned to traffic and wood burning sources using a model based on Published by Copernicus Publications on behalf of the European Geosciences Union. 962 M. Crippa et al.: The organic fraction in the metropolitan area of Paris wavelength-dependent light absorption of these two combustion sources. The time series of organic and black carbon factors from related sources were strongly correlated. The similarities in aerosol composition, total mass and temporal variation between the three sites suggest that particulate pollution in Paris is dominated by regional factors, and that the emissions from Paris itself have a relatively low impact on its surroundings.

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 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.DOI: 10.1034/j.1600-0889.1996.t01-1-00006.x

Large quantities of mineral dust particles are frequently ejected into the atmosphere through the action of wind. The surface of dust particles acts as a sink for many gases, such as sulfur dioxide. It is well known that under most conditions, sulfur dioxide reacts on dust particle surfaces, leading to the production of sulfate ions. In this report, for specific atmospheric conditions, we provide evidence for an alternate pathway in which a series of reactions under solar UV light produces first gaseous sulfuric acid as an intermediate product before surface-bound sulfate. Metal oxides present in mineral dust act as atmospheric photocatalysts promoting the formation of gaseous OH radicals, which initiate the conversion of SO 2 to H 2 SO 4 in the vicinity of dust particles. Under low dust conditions, this process may lead to nucleation events in the atmosphere. The laboratory findings are supported by recent field observations near Beijing, China, and Lyon, France.

Integrating nephelometers are in widespread use for measuring the particle scattering and hemispheric backscattering coefficients. Drawbacks of the nephelometer design are the truncation error and the non-lambertian illumination by the light source. In order to derive thescattering coefficient, data from nephelometers must be corrected for truncation and illumination errors. Corrections can be calculated using scattering theory if the particle size distribution and refractive index are known. If the particle shape differs from spheres, this method is not applicable.A new correctionbased on polar measurements was developed for the nephelometer Aurora4000.&nbsp

Background Although short-term exposure to ambient particulate matter has increasingly been linked with cardiovascular diseases, it is not quite clear how physical characteristics of particles, such as particle size may be responsible for the association. This study aimed at investigating whether daily changes in number or mass concentrations of accurately size-segregated particles in the range of 3 nm–10 μm are associated with daily cardiovascular emergency room visits in Beijing, China. Methods Cardiovascular emergency room visit counts, particle size distribution data, and meteorological data were collected from Mar. 2004 to Dec. 2006. Particle size distribution data was used to calculate particle number concentration in different size fractions, which were then converted to particle mass concentration assuming spherical particles. We applied a time-series analysis approach. We evaluated lagged associations between cardiovascular emergency room visits and particulate number and mass concentration using distributed lag non-linear models up to lag 10. We calculated percentage changes of cardiovascular emergency room visits, together with 95% confidence intervals (CI), in association with an interquartile range (IQR, difference between the third and first quartile) increase of 11-day or 2-day moving average number or mass concentration of particulate matter within each size fraction, assuming linear effects. We put interaction terms between season and 11-day or 2-day average particulate concentration in the models to estimate the modification of the particle effects by season. Results We observed delayed associations between number concentration of ultrafine particles and cardiovascular emergency room visits, mainly from lag 4 to lag 10, mostly contributed by 10–30 nm and 30–50 nm particles. An IQR (9040 cm −3 ) increase in 11-day average number concentration of ultrafine particles was associated with a 7.2% (1.1–13.7%) increase in total, and a 7.9% (0.5–15.9%) increase in severe cardiovascular emergency room visits. The delayed effects of particulate mass concentration were small. Regarding immediate effects, 2-day average number concentration of Aitken mode (30–100 nm) particles had strongest effects. An IQR (2269 cm −3 ) increase in 2-day average number concentration of 30–50 nm particles led to a 2.4% (−1.5–6.5%) increase in total, and a 1.7% (−2.9–6.5%) increase in severe cardiovascular emergency room visits. The immediate effects of mass concentration came mainly from 1000–2500 nm particles. An IQR (11.7 μg m −3 ) increase in 2-day average mass concentration of 1000–2500 nm particles led to an around 2.4% (0.4–4.4%) increase in total, and a 1.7% (−0.8–4.2%) increase in severe cardiovascular emergency room visits. The lagged effect curves of number and mass concentrations of 100–300 nm particles or 300–1000 nm particles were quite similar, indicating that using particulate number or mass concentrations seemed not to affect the cardiovascular effect (of particles within one size fraction). The effects of number concentration of ultrafine particles, sub-micrometer particles (3–1000 nm) and 10–30 nm particles were substantially higher in winter comparing with in summer. Conclusions Elevated concentration levels of sub-micrometer particles were associated with increased cardiovascular morbidity. Ultrafine particles showed delayed effects, while accumulation mode (100–1000 nm) particles showed immediate effects. Using number or mass concentrations did not affect the particle effects.

A three-dimensional regional chemical transport model (CTM) with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional (TOMAS) algorithm to track both aerosol number and mass concentration using a sectional approach. The model predicts nucleation events that occur over scales of hundreds up to thousands of kilometers especially over the Balkans and Southeast Europe. The model predictions were compared against measurements from 7 sites across Europe. The model reproduces more than 70% of the hourly concentrations of particles larger than 10 nm (N10) within a factor of 2. About half of these particles are predicted to originate from nucleation in the lower troposphere. Regional nucleation is predicted to increase the total particle number concentration by approximately a factor of 3. For particles larger than 100 nm the effect varies from an increase of 20% in the eastern Mediterranean to a decrease of 20% in southern Spain and Portugal resulting in a small average increase of around 1% over the whole domain. Nucleation has a significant effect in the predicted N50 levels (up to a factor of 2 increase) mainly in areas where there are condensable vapors to grow the particles to larger sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization performs better than the activation or the kinetic parameterizations in reproducing the observations. Reducing emissions of ammonia and sulfur dioxide affects certain parts of the number size distribution.

An Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed to investigate the size-resolved chemical composition of single particles at an urban background site in Paris, France, as part of the MEGAPOLI winter campaign in January/February 2010. ATOFMS particle counts were scaled to match coincident Twin Differential Mobility Particle Sizer (TDMPS) data in order to generate hourly size-resolved mass concentrations for the single particle classes observed. The total scaled ATOFMS particle mass concentration in the size range 150–1067 nm was found to agree very well with the sum of concurrent High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and Multi-Angle Absorption Photometer (MAAP) mass concentration measurements of organic carbon (OC), inorganic ions and black carbon (BC) (R2 = 0.91). Clustering analysis of the ATOFMS single particle mass spectra allowed the separation of elemental carbon (EC) particles into four classes: (i) EC attributed to biomass burning (ECbiomass), (ii) EC attributed to traffic (ECtraffic), (iii) EC internally mixed with OC and ammonium sulfate (ECOCSOx), and (iv) EC internally mixed with OC and ammonium nitrate (ECOCNOx). Average hourly mass concentrations for EC-containing particles detected by the ATOFMS were found to agree reasonably well with semi-continuous quantitative thermal/optical EC and optical BC measurements (r2 = 0.61 and 0.65–0.68 respectively, n = 552). The EC particle mass assigned to fossil fuel and biomass burning sources also agreed reasonably well with BC mass fractions assigned to the same sources using seven-wavelength aethalometer data (r2 = 0.60 and 0.48, respectively, n = 568). Agreement between the ATOFMS and other instrumentation improved noticeably when a period influenced by significantly aged, internally mixed EC particles was removed from the intercomparison. 88% and 12% of EC particle mass was apportioned to fossil fuel and biomass burning respectively using the ATOFMS data compared with 85% and 15% respectively for BC estimated from the aethalometer model. On average, the mass size distribution for EC particles is bimodal; the smaller mode is attributed to locally emitted, mostly externally mixed EC particles, while the larger mode is dominated by aged, internally mixed ECOCNOx particles associated with continental transport events. Periods of continental influence were identified using the Lagrangian Particle Dispersion Model (LPDM) "FLEXPART". A consistent minimum between the two EC mass size modes was observed at approximately 400 nm for the measurement period. EC particles below this size are attributed to local emissions using chemical mixing state information and contribute 79% of the scaled ATOFMS EC particle mass, while particles above this size are attributed to continental transport events and contribute 21% of the EC particle mass. These results clearly demonstrate the potential benefit of monitoring size-resolved mass concentrations for the separation of local and continental EC emissions. Knowledge of the relative input of these emissions is essential for assessing the effectiveness of local abatement strategies.

Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data., JRC.H.2-Air and Climate

We report on aerosol particles formed by bubbling a carrier gas through bubblers in metalorganic vapor phase epitaxy (MOVPE). A triethylgallium bubbler was investigated in a MOVPE set-up regarding the generation of aerosol. We measured particle number concentrations with an ultrafine condensation particle counter, which can detect submicrometer aerosol particles larger than 3 nm in diameter. We found that a standard triethylgallium bubbler used in a conventional way produces aerosol particles. The number of particles is a function of the carrier gas flow through the bubbler and correlates with the number of bubbles. The aerosol size distributions were analyzed with a differential mobility particle sizer and found to range from 10 to 600 nm, with maxima between 150 and 200 nm. Size distribution as well as total number of aerosol particles depend on evaporation processes during transport in undersaturated gas flows. While the number of particles reaching the reactor is not negligible, the precursor is predominantly transported as gas molecules. Particles can in principle, though, reach the substrate and create defects on the surface.

During a field measuring campaign at Kleiner Feldberg (Taunus) in 1990, microphysical characteristics of clouds have been measured by Forward Scattering Spectrometer Probes (FSSP). The aim was to study the influence of aerosol and meteorological factors on droplet size and number. The results are: More mass in the accumulation size range of the aerosol leads to more droplets in stratocumulus clouds and to higher soluble masses in droplets of stratus clouds. However, the aerosol distribution was coarser in the stratus clouds compared to the stratocumulus clouds. Within the first 200 m from cloud base, the droplets grow while their number decreases. The growth results in a stable size of about 14 µm diameter over a large distance from cloud base in many stratocumulus clouds. Two types of mixing processes were observed: processes with reductions in the number of droplets (inhomogeneous mixing) and with reductions in the size of the droplets (homogeneous mixing).

The partitioning of aerosol particles between cloud droplets and interstitial air by number and volume was determined both in terms of an integral value and as a function of size for clouds on Mt. Kleiner Feldberg (825 m asl), in the Taunus Mountains north-west of Frankfurt am Main, Germany. Differences in the integral values and the size dependent partitioning between two periods during the campaign were observed. Higher number and volume concentrations of aerosol particles in the accumulation mode were observed during Period II compared to Period I. In Period I on average 87 ± 11% (±one standard deviation) and 73 ± 7% of the accumulation mode volume and number were incorporated into cloud droplets. For Period II the corresponding fractions were 42 ± 6% and 12 ± 2% in one cloud event and 64 ± 4% and 18 ± 2% in another cloud event. The size dependent partitioning as a function of time was studied in Period II and found to have little variation. The major processes influencing the partitioning were found to be nucleation scavenging and entrainment.

An overview is given of the Kleiner Feldberg cloud experiment performed from 27 October until 13 November 1990. The experiment was carried out by numerous European research groups as a joint effort within the EUROTRAC-GCE project in order to study the interaction of cloud droplets with atmospheric trace constituents. After a description of the observational site and the measurements which were performed, the general cloud formation mechanisms encountered during the experiment are discussed. Special attention is given here to the process of moist adiabatic lifting. Furthermore, an overview is given regarding the pollutant levels in the gas phase, the particulate and the liquid phase, and some major findings are presented with respect to the experimental objectives. Finally, a first comparison attempts to put the results obtained during this campaign into perspective with the previous GCE field campaign in the Po Valley.

In the atmosphere, cloud and fog droplets usually contain insoluble material. The role of these insoluble particles is still unknown today, and is of interest to study. To determine the size distribution and number concentration of these particles in water, different techniques are available. The instrumentation, however, to measure nanometer-sized particles down to 50 nm diameter is not known. A new instrument, the Liquid Tandem Differential Mobility Analyser (LTDMA), was developed to measure size distributions of insoluble particles in water in the size range 50–300 nm in diameter. The new method is based on nebulising, e.g. cloud water and forming a residue aerosol consisting of both, insoluble particles with a soluble shell, and pure soluble particles. The insoluble, hydrophobic particles can be separated from soluble, hygroscopic residue particles with a Tandem Differential Mobility Analyser. The system is calibrated with monodisperse latex particles to determine the size-dependent transmission factor of insoluble particles of the Liquid Tandem Differential Mobility Analyser. A size distribution of insoluble particles in cloud water is presented as an application of this new measuring method. The cloud water sample was taken during the field campaign of the EUROTRAC sub project Ground-based Cloud Experiments (GCE) on the Kleiner Feldberg mountain, Germany, in November 1990.

Four different methods for measuring ultrafine particle size distributions in the 3–10-nm particle diameter range are compared and discussed. These methods all use an ultrafine condensation particle counter (TSI Inc. Model 3025 or its prototype) as the detector, but use different approaches to determine the size of the particles counted. Size classification was achieved using a Hauke Model VIE-06 differential mobility analyzer, a specially configured TSI Model 3040S diffusion battery, an ultrafine condensation particle counter with a variable condenser temperature, and an ultrafine condensation particle counter with a pulse height analyzer for signals produced by the optical detector. The response of these systems to ultrafine particles of known size and composition was studied during a workshop held in Lund, Sweden, during July 1991. After this workshop, measurements of ultrafine particles were made on the Swedish icebreaker Oden during the International Arctic Ocean Expedition 1991 (August 1, 1991 throu...

Measurements with two Raman-depolarization lidars of the Meteorological Institute of the Ludwig-Maximilians-Universitat, Munchen, 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 υ d 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 υ d > 95%. During the second phase, the AOD in the PBL was considerably lower and υ d 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. DOI: 10.1111/j.1600-0889.2011.00557.x

The regional dust model system LM-MUSCAT-DES was developed in the framework of the SAMUM project. Using the unique comprehensive data set of near-source dust properties during the 2006 SAMUM field campaign, the performance of the model system is evaluated for two time periods in May and June 2006. Dust optical thicknesses, number size distributions and the position of the maximum dust extinction in the vertical profiles agree well with the observations. However, the spatio-temporal evolution of the dust plumes is not always reproduced due to inaccuracies in the dust source placement by the model. While simulated winds and dust distributions are well matched for dust events caused by dry synoptic-scale dynamics, they are often misrepresented when dust emissions are caused by moist convection or influenced by small-scale topography that is not resolved by the model. In contrast to long-range dust transport, in the vicinity of source regions the model performance strongly depends on the correct prediction of the exact location of sources. Insufficiently resolved vertical grid spacing causes the absence of inversions in the model vertical profiles and likely explains the absence of the observed sharply defined dust layers.DOI: 10.1111/j.1600-0889.2008.00387.x

The present study covers submicrometer aerosol size distribution data taken during three Arctic icebreaker expeditionsin the summers of 1991, 1996 and 2001. The size distributions of all expeditions were compared in log-normally fittedform to the statistics of the marine number size distribution provided by Heintzenberg et al. (2004) yielding rather similarlog-normal parameters of the modes. Statistics of the modal concentrations revealed strong concentration decreases oflarge accumulation mode particles with increasing length of time spent over the pack ice. The travel-time dependenciesof both Aitken and ultrafine modes strongly indicate, as other studies did before, the occurrence of fine-particle sourcesin the inner Arctic.With two approaches evidence of fog-related aerosol source processeswas sought for in the data sets of 1996 and 2001because they included fog drop size distributions. With increasing fog intensity modes in interstitial particle numberconcentrations appeared in particular in the size range around 80 nm that was nearly mode free in clear air.A second, dynamic approach revealed that Aitken mode concentrations increased strongly above their respectivefog-period medians in both years before maximum drop numbers were reached in both years. We interpret the resultsof both approaches as strong indications of fog-related aerosol source processes as discussed in Leck and Bigg (1999)that need to be elucidated with further data from dedicated fog experiments in future Arctic expeditions in order tounderstand the life cycle of the aerosol over the high Arctic pack ice area.DOI: 10.1111/j.1600-0889.2005.00171.x

Submicrometre dry number size distributions from four marine and one continental aerosol experiment were evaluatedjointly in the present study. In the marine experiments only data with back trajectories of at least 120 h without landcontact were used to minimize continental contamination. Log-normal functions were fitted to the size distributions.Basic statistics of the marine aerosol indicate a closed character of the size distribution at the lower size limit as opposedto an open character for corresponding continental data. Together with the infrequent occurrences of marine particlesbelow20 nmthis finding supports hypotheses and model results suggesting lowprobabilities of homogeneous nucleationin the marine boundary layer. The variability of submicrometre marine number concentrations was parametrized witha bimodal log-normal function that quantifies the probability of finding different number concentrations about a givenmedian value. Together with a four-modal log-normal approximation of the submicrometre marine size distributionitself, this model allows a statistical representation of the marine aerosol that facilitates comparison of experiments andvalidation of aerosol models. Autocorrelation at the one fixed marine site with a minimum of interruptions in timesseriesrevealed a strong size dependency of persistence in particle number concentration with the shortest persistenceat the smallest sizes. Interestingly, in the marine aerosol (at Cape Grim) persistence exhibits a size dependency thatlargely matches the modes in dg0, i.e. near the most frequent geometric mean diameters number concentrations aremost persistent. Over the continent, persistence of particle numbers is strongly constrained by diurnal meteorologicalprocesses and aerosol dynamics. Thus, no strong modal structure appears in the size-dependent persistence at Melpitz.As with the aerosol variability, marine aerosol processes in models of aerosol dynamics can be tested with these findings. DOI: 10.1111/j.1600-0889.2004.00115.x

A large field experiment of the Saharan Mineral Dust Experiment (SAMUM) was performed in Praia, Cape Verde, in January and February 2008. This work reports on the aerosol mass concentrations, size distributions and mineralogical composition of the aerosol arriving at Praia. Three dust periods were recorded during the measurements, divided by transitional periods and embedded in maritime-influenced situations. The total suspended particle mass/PM 10 /PM 2.5 were 250/180/74 μg/m 3 on average for the first dust period (17–21 January) and 250/230/83 μg/m 3 for the second (24–26 January). The third period (28 January to 2 February) was the most intensive with 410/340/130 μg/m 3 . Four modes were identified in the size distribution. The first mode (50–70 nm) and partly the second (700–1100 nm) can be regarded as of marine origin, but some dust contributes to the latter. The third mode (2–4 μm) is dominated by advected dust, while the intermittently occurring fourth mode (15–70 μm) may have a local contribution. The dust consisted of kaolinite (dust/maritime period: 35%wt./25%wt.), K-feldspar (20%wt./25%wt.), illite (14%wt./10%wt.), quartz (11%wt./8%wt.), smectites (6%wt./4%wt.), plagioclase (6%wt./1%wt.), gypsum (4%wt./7%wt.), halite (2%wt./17%wt.) and calcite (2%wt./3%wt.). DOI: 10.1111/j.1600-0889.2011.00546.x

Past studies have indicated that long-term averages of the aerosol number to volume ratios (defined as the number ofparticles larger than a certain diameter divided by the particle volume over some range less than 1 μm) show littlevariability over the Atlantic. This work presents number to volume ratios (R) measured during the ACE-2 experiment onthe land-based Sagres field site located in Southwest Portugal. The values of R measured in Sagres compare reasonablywell with previous measurements over the Atlantic. The main emphasis of this work is therefore to investigate moreclosely possible reasons for the observed stability of the number to volume ratio. Aerosol number size distributionsmeasured in Sagres are parametrized by the sum of two log-normal distributions fitted to the accumulation and to theAitken mode. The main factor that limits the variability of R is that the parameters of these log-normal distributionsare not always independent but show some covariance. In polluted air mass types correlations between parameters ofthe Aitken and accumulation mode are mostly responsible for stabilizing R. In marine air mass types the variabilityof 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 concentrationof particles larger than 90 nm. This partly due to a tail of Aitken-mode particles extending to sizes larger than90 nm. DOI: 10.1111/j.1600-0889.2004.00119.x

During the SATURN campaign 2002, new particle formation, i.e. the occurrence of ultrafine particles was investigated simultaneously at four ground-based measurement sites. The maximum distance between the sites was 50 km. Additionally, vertical profiles of aerosol particles from 5–10 nm have been measured by a tethered-balloon-borne system at one of the sites. In general, two different scenarios have been found: (i) new particle formation was measured at all sites nearly in parallel with subsequent particle growth (homogeneous case) and (ii) new particle formation was observed at one to three sites irregularly (inhomogeneous case) where subsequent particle growth was often interrupted. The homogeneous case was connected with stable synoptical conditions, i.e. the region was influenced by a high pressure system. Here, the horizontal extent of the phenomenon has been estimated to be 400 km at maximum. In the vertical dimension, the ultrafine particles are well mixed within the entire boundary layer. In the inhomogeneous case the new particle formation depends mainly on the incoming solar radiation and was often interrupted due the occurrence of clouds. Thus, single point measurements are not representative for a larger region in that case. DOI: 10.1111/j.1600-0889.2007.00260.x

The difference in chemistry between interstitial aerosol particles and particles that were scavenged into fog droplets is examined using multivariate statistical techniques. 15 trace elements (P, S, Cl, K, Ca, Cr, Mn, Fe, Ni, Cu, Zn, Se, Br, Pb, EC) were used in the analysis. There was a significant difference in composition between the two types of particles. S, Fe, Mn, and Cu were among the elements best describing the scavenged aerosol, while the interstitial aerosol was best described by elemental carbon (EC). DOI: 10.1034/j.1600-0889.1992.t01-1-00011.x

Aerosol physics measurements made onboard the Swedish icebreaker Oden in the late Summer and early Autumn of 1991 during the International Arctic Ocean Expedition (IAOE-91) have provided the first data on the size distribution of particles in the Arctic marine boundary layer (MBL) that cover both the number and mass modes of the size range from 3 to 500 nm diameter. These measurements were made in conjunction with atmospheric gas and condensed phase chemistry measurements in an effort to understand a part of the ocean-atmosphere sulphur cycle. Analysis of the particle physics data showed that there were three distinct number modes in the submicrometric aerosol in the Arctic MBL. These modes had geometric mean diameters of around 170 nm, 45 nm and 14 nm referred to as accumulation, Aitken and ultrafine modes, respectively. There were clear minima in number concentrations between the modes that appeared at 20–30 nm and at 80–100 nm. The total number concentration was most frequently between 30 and 60 particles cm −3 with a mean value of around 100 particles cm −3 , but the hourly average concentration varied over two to three orders of magnitude during the 70 days of the expedition. On average, the highest concentration was in the accumulation mode that contained about 45% of the total number, while the Aitken mode contained about 40%. The greatest variability was in the ultrafine mode concentration which is indicative of active, nearby sources (nucleation from the gas phase) and sinks; the Aitken and accumulation mode concentrations were much less variable. The ultrafine mode was observed about two thirds of the time and was dominant 10% of the time. A detailed description and statistical analysis of the modal aerosol parameters is presented here. DOI: 10.1034/j.1600-0889.1996.t01-1-00005.x

Measurements of the scavenging efficiency of aerosol particles in fog are presented. The scavenging efficiency as a function of size for accumulation-mode particles is presented, along with efficiencies for the total number, accumulation-mode number, and accumulation-mode volume. Particles below ca. 0.3 µ m diameter were not efficiently scavenged in the fogs. The scavenging efficiency for accumulation-mode particles showed two steps, indicating that the hygroscopic/hydrophobic nature of the aerosol appeared to have been a controlling factor in determining scavenging efficiencies. Observed changes in the aerosol size distributions are discussed in reference to the processes (i.e., in-cloud scavenging, aqueous-phase reactions) potentially influencing them. DOI: 10.1034/j.1600-0889.1992.t01-4-00004.x

Soot particles are regarded as the most efficient light absorbing aerosol species in the atmosphere, playing an important role as a driver of global warming. Their climate effects strongly depend on their mixing state, which significantly changes their light absorbing capability and cloud condensation nuclei (CCN) activity. Therefore, knowledge about the mixing state of soot and its aging mechanism becomes an important topic in the atmospheric sciences. The size-resolved (30–320 nm diameter) mixing state of soot particles in polluted megacity air was measured at a suburban site (Yufa) during the CAREBeijing 2006 campaign in Beijing, using a Volatility Tandem Differential Mobility Analyzer (VTDMA). Particles in this size range with non-volatile residuals at 300 °C were considered to be soot particles. On average, the number fraction of internally mixed soot in total soot particles (Fin), decreased from 0.80 to 0.57 when initial Dp increased from 30 nm to 320 nm. Further analysis reveals that: (1) Fin was well correlated with the aerosol hygroscopic mixing state measured by a CCN counter. More externally mixed soot particles were observed when particles showed more heterogeneous features with regard to hygroscopicity. (2) Fin had pronounced diurnal cycles. For particles in the accumulation mode (Dp at 100–320 nm), largest Fin were observed at noon time, with apparent turnover rates (kex → in) up to 7.8% h−1. (3) Fin was subject to competing effects of both aging and emissions. While aging increases Fin by converting externally mixed soot particles into internally mixed ones, emissions tend to reduce Fin by emitting more fresh and externally mixed soot particles. Similar competing effects were also found with air mass age indicators. (4) Under the estimated emission intensities, actual turnover rates of soot (kex → in) up to 20% h−1 were derived, which showed a pronounced diurnal cycle peaking around noon time. This result confirms that (soot) particles are undergoing fast aging/coating with the existing high levels of condensable vapors in the megacity Beijing. (5) Diurnal cycles of Fin were different between Aitken and accumulation mode particles, which could be explained by the faster size shift of smaller particles in the Aitken mode. To improve the Fin prediction in regional/global models, we suggest parameterizing Fin by an air mass aging indicator, i.e., Fin = a + bx, where a and b are empirical coefficients determined from observations, and x is the value of an air mass age indicator. At the Yufa site in the North China Plain, fitted coefficients (a, b) were determined as (0.57, 0.21), (0.47, 0.21), and (0.52, 0.0088) for x (indicators) as [NOz]/[NOy], [E]/[X] ([ethylbenzene]/[m,p-xylene]) and ([IM] + [OM])/[EC] ([inorganic + organic matter]/elemental carbon]), respectively. Such a parameterization consumes little additional computing time, but yields a more realistic description of Fin.

It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models., JRC.H.2-Air and Climate

Background and Aims: Numerous studies have shown associations between human health and air pollution or air temperature. Whether both exposures have synergistic effects on health outcomes has so fa...

The spatio-temporal evolution of the Saharan dust and biomass-burning plume during the SAMUM-2 field campaign in January and February 2008 is simulated at 28 km horizontal resolution with the regional model-system COSMO-MUSCAT. The model performance is thoroughly tested using routine ground-based and space-borne remote sensing and local field measurements. Good agreement with the observations is found in many cases regarding transport patterns, aerosol optical thicknesses and the ratio of dust to smoke aerosol. The model also captures major features of the complex aerosol layering. Nevertheless, discrepancies in the modelled aerosol distribution occur, which are analysed in detail. The dry synoptic dynamics controlling dust uplift and transport during the dry season are well described by the model, but surface wind peaks associated with the breakdown of nocturnal low-level jets are not always reproduced. Thus, a strong dust outbreak is underestimated. While dust emission modelling is a priori more challenging, since strength and placement of dust sources depend on on-line computed winds, considerable inaccuracies also arise in observation-based estimates of biomass-burning emissions. They are caused by cloud and spatial errors of satellite fire products and uncertainties in fire emission parameters, and can lead to unrealistic model results of smoke transport.DOI: 10.1111/j.1600-0889.2011.00570.x

Numerous studies have described the adverse associations between particle mass and respiratory health. The aim of the study was to analyze the associations of particle properties, especially size-segregated particle number concentrations (PNC), and respiratory mortality in Beijing, P.R. China. We gathered daily values of respiratory mortality and air pollution data of the Beijing urban area. Generalized additive models were used to estimate the associations. Single pollutant models showed that delayed concentrations of SO(2), total PNCs, and PNC of 300-1000 nm were adversely associated with total respiratory mortality. There was an indication that adverse health effects of PNCs might be stronger for stagnant air masses. Two-pollutant models verified the independence of associations of total PNCs of other pollutants (SO(2), NO(2), and PM(10)). In conclusion, particle number concentrations, especially accumulation mode particles, might be factors influencing the adverse associations between particulate matter and respiratory health.