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Proxies for estimating nucleation mode number concentrations and further simplification for their use with satellite data have been presented in Kulmala et al. (2011). In this paper we discuss the underlying assumptions for these simplifications and evaluate the resulting proxies over an area in South Africa based on a comparison with a suite of ground-based measurements available from four different stations. The proxies are formulated in terms of sources (concentrations of precursor gases (NO2 and SO2) and UVB radiation intensity near the surface) and a sink term related to removal of the precursor gases due to condensation on pre-existing aerosols. A-Train satellite data are used as input to compute proxies. Both the input data and the resulting proxies are compared with those obtained from ground-based measurements. In particular, a detailed study is presented on the substitution of the local condensation sink (CS) with satellite aerosol optical depth (AOD), which is a columnintegrated parameter. One of the main factors affecting the disagreement between CS and AOD is the presence of elevated aerosol layers. Overall, the correlation between proxies calculated from the in situ data and observed nucleation mode particle number concentrations (Nnuc) remained low. At the time of the satellite overpass (13:00–14:00 LT) the highest correlation is observed for SO2/CS (R2 D 0:2). However, when the proxies are calculated using satellite data, only NO2/AOD showed some correlation with Nnuc (R2 D 0:2). This can be explained by the relatively high uncertainties related especially to the satellite SO2 columns and by the positive correlation that is observed between the ground-based SO2 and NO2 concentrations. In fact, results show that the satellite NO2 columns compare better with in situ SO2 concentration than the satellite SO2 column. Despite the high uncertainties related to the proxies calculated using satellite data, the proxies calculated from the in situ data did not better predict Nnuc. Hence, overall improvements in the formulation of the proxies are needed http://www.atmos-chem-phys.net/15/4983/2015/ doi:10.5194/acp-15-4983-2015, 2015

South Africa has one of the largest industrialized economies in Africa. Emissions of air pollutants are particularly high in the Johannesburg-Pretoria metropolitan area, the Mpumalanga Highveld and the Vaal Triangle, resulting in local air pollution. This study presents and evaluates a setup for conducting modeling experiments over southern Africa with the Weather Research and Forecasting model including chemistry and aerosols (WRF-Chem), and analyzes the contribution of anthropogenic emissions to the total black carbon (BC) concentrations from September to December 2010. The modeled BC concentrations are compared with measurements obtained at the Welgegund station situated ca. 100 km southwest of Johannesburg. An evaluation of WRF-Chem with observational data from ground-based measurement stations, radiosondes, and satellites shows that the meteorology is modeled mostly reasonably well, but precipitation amounts are widely overestimated and the onset of the wet season is modeled approximately 1 month too early in 2010. Modeled daily mean BC concentrations show a temporal correlation of 0.66 with measurements, but the total BC concentration is underestimated in the model by up to 50 %. Sensitivity studies with anthropogenic emissions of BC and co-emitted species turned off show that anthropogenic sources can contribute up to 100% to BC concentrations in the industrialized and urban areas, and anthropogenic BC and co-emitted species together can contribute up to 60% to PM1 levels. Particularly the co-emitted species contribute significantly to the aerosol optical depth (AOD). Furthermore, in areas of large-scale biomass-burning atmospheric heating rates are increased through absorption by BC up to an altitude of about 600 hPa doi:10.5194/acp-15-8809-2015 http://www.atmos-chem-phys.net/15/8809/2015/

Raman lidar data obtained over a 1 year period has been analysed in relation to aerosol layers in the free troposphere over the Highveld in South Africa. In total, 375 layers were observed above the boundary layer during the period 30 January 2010 to 31 January 2011. The seasonal behaviour of aerosol layer geometrical characteristics, as well as intensive and extensive optical properties were studied. The highest centre heights of free-tropospheric layers were observed during the South African spring (2520 ± 970 m a.g.l., also elsewhere). The geometrical layer depth was found to be maximum during spring, while it did not show any significant difference for the rest of the seasons. The variability of the analysed intensive and extensive optical properties was high during all seasons. Layers were observed at a mean centre height of 2100 ± 1000 m with an average lidar ratio of 67 ± 25 sr (mean value with 1 standard deviation) at 355 nm and a mean extinction-related Ångström exponent of 1.9 ± 0.8 between 355 and 532 nm during the period under study. Except for the intensive biomass burning period from August to October, the lidar ratios and Ångström exponents are within the range of previous observations for urban/industrial aerosols. During Southern Hemispheric spring, the biomass burning activity is clearly reflected in the optical properties of the observed free-tropospheric layers. Specifically, lidar ratios at 355 nm were 89 ± 21, 57 ± 20, 59 ± 22 and 65 ± 23 sr during spring (September–November), summer (December–February), autumn (March–May) and winter (June–August), respectively. The extinction-related Ångström exponents between 355 and 532 nm measured during spring, summer, autumn and winter were 1.8 ± 0.6, 2.4 ± 0.9, 1.8 ± 0.9 and 1.8 ± 0.6, respectively. The mean columnar aerosol optical depth (AOD) obtained from lidar measurements was found to be 0.46 ± 0.35 at 355 nm and 0.25 ± 0.2 at 532 nm. The contribution of free-tropospheric aerosols on the AOD had a wide range of values with a mean contribution of 46% http://www.atmos-chem-phys.net/15/5429/2015/ doi:10.5194/acp-15-5429-2015, 2015

Southern Africa is a significant source region of atmospheric pollution, yet long-term data on pollutant concentrations and properties from this region are rather limited. A recently established atmospheric measurement station in South Africa, Welgegund, is strategically situated to capture regional background concentrations, as well as emissions from the major source regions in the interior of South Africa. We measured non-refractive submicron aerosols (NR-PM1) and black carbon over a one year period in Welgegund, and investigated the seasonal and diurnal patterns of aerosol concentration levels, chemical composition, acidity and oxidation level. Based on air mass back trajectories, four distinct source regions were determined for NR-PM1. Supporting data utilised in our analysis included particle number size distributions, aerosol absorption, trace gas concentrations, meteorological variables and the flux of carbon dioxide. The dominant submicron aerosol constituent during the dry season was organic aerosol, reflecting high contribution from savannah fires and other combustion sources. Organic aerosol concentrations were lower during the wet season, presumably due to wet deposition as well as reduced emissions from combustion sources. Sulfate concentrations were usually high and exceeded organic aerosol concentrations when air-masses were transported over regions containing major point sources. Sulfate and nitrate concentrations peaked when air masses passed over the industrial Highveld (iHV) area. In contrast, concentrations were much lower when air masses passed over the cleaner background (BG) areas. Air masses associated with the anti-cyclonic recirculation (ACBIC) source region contained largely aged OA. Positive Matrix Factorization (PMF) analysis of aerosol mass spectra was used to characterise the organic aerosol (OA) properties. The factors identified were oxidized organic aerosols (OOA) and biomass burning organic aerosols (BBOA) in the dry season and low-volatile (LV-OOA) and semi-volatile (SV-OOA) organic aerosols in the wet season. The results highlight the importance of primary BBOA in the dry season, which represented 33% of the total OA. Aerosol acidity and its potential impact on the evolution of OOA are also discussed http://dx.doi.org/10.5194/acp-14-1909-2014 http://www.atmospheric-chemistry-and-physics.net/ Finnish Academy (Atmospheric monitoring capacity building in Southern Africa: project no. 132640), the Saastamoinen foundation, as well as support from the North-West University and the Finnish Meteorological Institute. Academy of Finland Centre of Excellence program

Atmospheric lidar measurements were carried out at Elandsfontein measurement station, on the eastern Highveld approximately 150 km east of Johannesburg in South Africa throughout 2010. The height of the planetary boundary layer (PBL) top was continuously measured using a Raman lidar, PollyXT (POrtabLe Lidar sYstem eXTended). High atmospheric variability together with a large surface temperature range and significant seasonal changes in precipitation were observed, which had an impact on the vertical mixing of particulate matter, and hence, on the PBL evolution. The results were compared to radiosondes, CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) spaceborne lidar measurements and three atmospheric models that followed different approaches to determine the PBL top height. These models included two weather forecast models operated by ECMWF (European Centre for MediumrangeWeather Forecasts) and SAWS (South AfricanWeather Service), and one mesoscale prognostic meteorological and air pollution regulatory model TAPM (The Air Pollution Model). The ground-based lidar used in this study was operational for 4935 h during 2010 (49% of the time). The PBL top height was detected 86% of the total measurement time (42% of the total time). Large seasonal and diurnal variations were observed between the different methods utilised. High variation was found when lidar measurements were compared to radiosonde measurements. This could be partially due to the distance between the lidar measurements and the radiosondes, which were 120 km apart. Comparison of lidar measurements to the models indicated that the ECMWF model agreed the best with mean relative difference of 15.4 %, while the second best correlation was with the SAWS model with corresponding difference of 20.1 %. TAPM was found to have a tendency to underestimate the PBL top height. The wind speeds in the SAWS and TAPM models were strongly underestimated which probably led to underestimation of the vertical wind and turbulence and thus underestimation of the PBL top height. Comparison between ground-based and satellite lidar shows good agreement with a correlation coefficient of 0.88. On average, the daily maximum PBL top height in October (spring) and June (winter) was 2260m and 1480 m, respectively. To our knowledge, this study is the first long-term study of PBL top heights and PBL growth rates in South Africa http://dx.doi.org/10.5194/acp-14-4263-2014 http://www.atmospheric-chemistry-and-physics.net/ Partly supported by the European Union (in project EUCAARI)

Aromatic hydrocarbons are associated with direct adverse human health effects and can have negative impacts on ecosystems due to their toxicity, as well as indirect negative effects through the formation of tropospheric ozone and secondary organic aerosol, which affect human health, crop production and regional climate. Measurements of aromatic hydrocarbons were conducted at the Welgegund measurement station (South Africa), which is considered to be a regionally representative background site. However, the site is occasionally impacted by plumes from major anthropogenic source regions in the interior of South Africa, which include the western Bushveld Igneous Complex (e.g. platinum, base metal and ferrochrome smelters), the eastern Bushveld Igneous Complex (platinum and ferrochrome smelters), the Johannesburg–Pretoria metropolitan conurbation (>10 million people), the Vaal Triangle (e.g. petrochemical and pyrometallurgical industries), the Mpumalanga Highveld (e.g. coal-fired power plants and petrochemical industry) and also a region of anticyclonic recirculation of air mass over the interior of South Africa. The aromatic hydrocarbon measurements were conducted with an automated sampler on Tenax- TA and Carbopack-B adsorbent tubes with heated inlet for 1 year. Samples were collected twice a week for 2 h during daytime and 2 h during night-time. A thermal desorption unit, connected to a gas chromatograph and a mass selective detector was used for sample preparation and analysis. Results indicated that the monthly median (mean) total aromatic hydrocarbon concentrations ranged between 0.01 (0.011) and 3.1 (3.2) ppb. Benzene levels did not exceed the local air quality standard limit, i.e. annual mean of 1.6 ppb. Toluene was the most abundant compound, with an annual median (mean) concentration of 0.63 (0.89) ppb. No statistically significant differences in the concentrations measured during daytime and night-time were found, and no distinct seasonal patterns were observed. Air mass back trajectory analysis indicated that the lack of seasonal cycles could be attributed to patterns determining the origin of the air masses sampled. Aromatic hydrocarbon concentrations were in general significantly higher in air masses that passed over anthropogenically impacted regions. Inter-compound correlations and ratios gave some indications of the possible sources of the different aromatic hydrocarbons in the source regions defined in the paper. The highest contribution of aromatic hydrocarbon concentrations to ozone formation potential was also observed in plumes passing over anthropogenically impacted regions http://dx.doi.org/10.5194/acp-14-7075-2014 http://www.atmospheric-chemistry-and-physics.net/ Finnish Academy (project no. 132640), the University of Helsinki, the Finnish Meteorological Institute and the North-West University

Absorption Ångström exponents (AAEs) calculated from filter-based absorption measurements are often used to give information on the origin of the ambient aerosol, for example, to distinguish between urban pollution and biomass burning aerosol. Filter-based absorption measurements are widely used and are common at aerosol monitoring stations globally. Several correction algorithms are used to account for artefacts associated with filter-based absorption techniques. These algorithms are of profound importance when determining the absolute amount of absorption by the aerosol. However, this study shows that there are substantial differences between the AAEs calculated from these corrections. Depending on the used correction, AAEs can change by as much as 46 %. The study also highlights that the difference between AAEs calculated using different corrections can lead to conflicting conclusions on the type of aerosol when using the same data set. The AAE ranged between 1.17 for non-corrected data to 1.96 for the correction that gave the greatest values. Furthermore, the study implies that the AAEs reported for a site depend on at which filter transmittance the filter is changed. In this work, the AAEs were calculated from data measured with a three-wavelength particle soot absorption photometer (PSAP) at Elandsfontein on the South African Highveld for 23 months. The sample air of the PSAP was diluted to prolong filter change intervals, by a factor of 15. The correlation coefficient between the dilution-corrected PSAP and a non-diluted Multi-Angle Absorption Photometer (MAAP) was 0.9. Thus, the study also shows that the applicability of the PSAP can be extended to remote sites that are not often visited or suffer from high levels of pollution http://www.atmospheric-measurement-techniques.net/ http:dx.doi.org/10.5194/amt-7-4285-2014 European commission 6th Framework programme project EUCAARI. Academy of Finland Centre of Excellence program (project nos. 1118615 and 272041). Eskom and Sasol Ltd.

Aerosol particles from shipping emissions both cool the climate and cause adverse health effects. The cooling effect is, however, declining because of shipping emission controls aiming to improve air quality. We used an aerosol-climate model ECHAM-HAMMOZ to test whether by altering ship fuel sulfur content, the present-day aerosol-induced cooling effect from shipping could be preserved, while at the same time reducing premature mortality rates related to shipping emissions. We compared the climate and health effects of a present-day shipping emission scenario (ship fuel sulfur content of 2.7%) with (1) a simulation with strict emission controls in the coastal waters (ship fuel sulfur content of 0.1%) and twofold the present-day fuel sulfur content (i.e. 5.4%) elsewhere; and (2) a scenario with global strict shipping emission controls (ship fuel sulfur content of 0.1% in coastal waters and 0.5% elsewhere) roughly corresponding to international agreements to be enforced by the year 2020. Scenario 1 had a slightly stronger aerosol-induced effective radiative forcing (ERF) from shipping than the present-day scenario (−0.43 W m−2 vs. −0.39 W m−2) while reducing premature mortality from shipping by 69% (globally 34 900 deaths avoided per year). Scenario 2 decreased the ERF to −0.06 W m−2 and annual deaths by 96% (globally 48 200 deaths avoided per year) compared to present-day. Our results show that the cooling effect of present-day emissions could be retained with simultaneous notable improvements in air quality, even though the shipping emissions from the open ocean clearly have a significant effect on continental air quality. However, increasing ship fuel sulfur content in the open ocean would violate existing international treaties, could cause detrimental side-effects, and could be classified as geoengineering. http://dx.doi.org/10.5194/acp-13-12059-2013 http://www.atmospheric-chemistry-and-physics.net/ http://www.atmos-chem-phys.net/13/issue23.html

The South African savannah region is a complex environment of air pollution and natural emissions influenced by a strong seasonal cycle in biomass burning and strong precipitation. However, the scarcity of long-term observations means that the knowledge of controlling aerosol processes in this environment is limited. Here we use a recent dataset of 18 months of aerosol size distribution observations trying to understand the annual cycle of cloud condensation nuclei (CCN). Our observations show that the concentration of CCN-sized particles remains, in line with previous studies, high throughout the year with the highest concentrations during the dry winter and the lowest during the wet summer. During the wet season with reduced anthropogenic and biomass burning primary emissions, this pool of CCN is partly filled by boundary layer nucleation with subsequent growth. The enhanced importance of formation and growth during the wet season is addressed to increased biogenic activity together with enhanced free tropospheric removal decreasing the concentration of pre-existing CCN. During the dry season, while frequent new particle formation takes place, particle growth is reduced due to reduced condensing vapour concentrations. Thus in the dry season particles are not able to grow to sizes where they may act as CCN nearly as efficiently as during the wet season. The observations are compared to simulations by a global aerosol model GLOMAP. To our surprise, the global aerosol model utilized to explain the observations was not capable of re-producing the characteristics of particle formation and the annual CCN cycle, despite earlier good performance in predicting the particle concentrations in a number of diverse environments, including the South African savannah region. While the average yearly CCN concentrations of modelled CCN is close to observed concentrations, the characteristics of nucleation bursts and subsequent growth are not captured satisfactory by the model. Our sensitivity tests using different nucleation parameterizations and condensing organic vapour production rates show that neither of these is likely to explain the differences between observed and modelled nucleation and growth rates. A sensitivity study varying 28 modelling parameters indicates that the main uncertainties in the result are due to uncertainties in biomass burning emissions during the dry season, and anthropogenic sulphur emissions during the wet season, both in terms or emitted mass and particle sizes. The uncertainties appear to be mostly related to uncertainties in primary particle emissions, including the emissions variability not captured by monthly emission inventories. The results of this paper also highlights the fact that deficiencies in emissions estimates may result in deficiencies in particle production fluxes, while the end product such as modelled CCN concentration may be in line with observations http://www.atmospheric-chemistry-and-physics.net/ http://www.atmospheric-chemistry-and-physics.net/ http://www.atmos-chem-phys.net/13/issue4.html http://dx.doi.org/10.5194/acp-13-1957-2013

The fraction of charged nucleation mode particles as a function of particle diameter depends on the particle growth rate and the proportion of particles formed via ion-induced nucleation. In this study we have tested the applicability of recent data analysis methods to determine the growth rate and the proportion of ion-induced nucleation from the measured charged fractions. For this purpose we have conducted a series of aerosol dynamic simulations covering a wide range of atmospheric conditions. The growth rate and initial fraction of charged particles were estimated from simulated data using these methods and compared with the values obtained directly from the simulations. We found that the data analysis methods used in this study should not be used when the nuclei growth rate is less than ~3 nm h−1, or when charged particles grow much more rapidly than neutral ones. Furthermore, we found that the difference in removal rates of neutral and charged particles should be taken into account when estimating the proportion of ion-induced nucleation. Neglecting the higher removal rate of charged particles compared with that of neutral ones could result in an underestimation of the proportion of ion-induced nucleation by up to a factor of 2. This underestimation is further increased if charged particles grow more rapidly than neutral ones. We also provided a simple way of assessing whether these methods are suitable for analyzing data measured under specific conditions. The assessment procedure was illustrated using a few examples of actual measurement sites with a more detailed examination of the typical conditions observed at the SMEAR II station in Hyytiälä, Finland. http://www.atmos-chem-phys.net/13/463/2013/acp-13-463-2013.html http://www.atmospheric-chemistry-and-physics.net/ http://dx.doi.org/10.5194/acp-13-463-2013

In this paper we introduce new in situ observations of atmospheric aerosols, especially chemical composition, physical and optical properties, on the eastern brink of the heavily polluted Highveld area in South Africa. During the observation period between 11 February 2009 and 31 January 2011, the mean particle number concentration (size range 10–840 nm) was 6310 cm3 and the estimated volume of sub-10 μm particles 9.3 μm3 m−3. The aerosol absorption and scattering coefficients at 637 nm were 8.3 Mm−1 and 49.5 Mm−1, respectively. The mean single-scattering albedo at 637 nm was 0.84 and the Ångström exponent of scattering was 1.5 over the wavelength range 450–635 nm. The mean O3, SO2, NOx and H2S-concentrations were 37.1, 11.5, 15.1 and 3.2 ppb, respectively. The observed range of concentrations was large and attributed to the seasonal variation of sources and regional meteorological effects, especially the anticyclonic re-circulation and strong winter-time inversions. In a global context, the levels of gases and particulates were typical for continental sites with strong anthropogenic influence, but clearly lower than the most polluted areas of south-eastern Asia. Of all pollutants observed at the site, ozone is the most likely to have adverse environmental effects, as the concentrations were high also during the growing season. The measurements presented here will help to close existing gaps in the ground-based global atmosphere observation system, since very little long-term data of this nature is available for southern Africa. http://dx.doi.org/10.5194/acp-12-1847-2012 http://www.atmos-chem-phys.net/12/1847/2012/acp-12-1847-2012.pdf

South Africa holds significant mineral resources, with a substantial fraction of these reserves occurring and being processed in a large geological structure termed the Bushveld Igneous Complex (BIC). The area is also highly populated by informal, semi-formal and formal residential developments. However, knowledge of air quality and research related to the atmosphere is still very limited in the area. In order to investigate the characteristics and processes affecting sub-micron particle number concentrations and formation events, air ion and aerosol particle size distributions and number concentrations, together with meteorological parameters, trace gases and particulate matter (PM) were measured for over two years at Marikana in the heart of the western BIC. The observations showed that trace gas (i.e. SO2, NOx, CO) and black carbon concentrations were relatively high, but in general within the limits of local air quality standards. The area was characterised by very high condensation sink due to background aerosol particles, PM10 and O3 concentration. The results indicated that high amounts of Aitken and accumulation mode particles originated from domestic burning for heating and cooking in the morning and evening, while during daytime SO2-based nucleation followed by the growth by condensation of vapours from industrial, residential and natural sources was the most probable source for large number concentrations of nucleation and Aitken mode particles. Nucleation event day frequency was extremely high, i.e. 86% of the analysed days, which to the knowledge of the authors is the highest frequency ever reported. The air mass back trajectory and wind direction analyses showed that the secondary particle formation was influenced both by local and regional pollution and vapour sources. Therefore, our observation of the annual cycle and magnitude of the particle formation and growth rates during nucleation events were similar to results previously published for a semi-clean savannah site in South Africa. http://dx.doi.org/10.5194/acp-12-3951-2012 http://www.atmos-chem-phys.net/12/3951/2012/acp-12-3951-2012.pdf

In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies. http://dx.doi.org/10.5194/acp-11-13061-2011 http://www.atmos-chem-phys.net/11/13061/2011/acp-11-13061-2011.pdf

We present the longest series of measurements so far (2 years and 7 months) made with an Ion-DMPS at the SMEAR II measurement station in Hyytiälä, Southern Finland. We show that the classification of overcharged (implying some participation of ion-induced nucleation) and undercharged (implying no or very little participation of ion-induced nucleation) days based on Ion-DMPS measurements agrees with the fraction of ion-induced nucleation based on NAIS measurements. We analyzed the influence of different parameters on the contribution of ion-induced nucleation to the total particle formation rate. We found that the fraction of ion-induced nucleation is typically higher on warmer, drier and sunnier days compared to colder days with less solar radiation and a higher relative humidity. Also, we observed that bigger concentrations of new particles were produced on days with a smaller fraction of ion-induced nucleation. Moreover, sulfuric acid concentrations were smaller for days with a bigger fraction of ion-induced nucleation. Finally, we propose tentative explanations on how these different parameters influence the different nucleation mechanisms, and show that the different mechanisms seem to take place at the same time during an event. The relative contribution of the different mechanisms seems to vary depending on the surrounding conditions.

http://dx.doi.org/10.5194/acpd-8-6313-2008

Biogenic aerosol formation is likely to contribute significantly to the global aerosol load. In recent years, new-particle formation (NPF) has been observed in various ecosystems around the world but hardly any measurements have taken place in the terrestrial Southern Hemisphere. Here, we report the first results of atmospheric ion and charged particle concentrations as well as of NPF in a Eucalypt forest in Tumbarumba, South-East Australia, from July 2005 to October 2006. The measurements were carried out with an Air Ion Spectrometer (AIS) with a size range from 0.34 to 40 nm. Daytime aerosol formation took place on 52% of days with acceptable data. Median growth rates (GR) for negative/positive 1.3–3 nm particles were 2.29/2.02 nmh−1; for 3–7 nm particles 3.04/2.94 nmh−1; and for 7–20 nm particles 7.13/5.62 nmh−1, respectively. Intermediate ion growth rates were highest when the wind was blowing from the direction of the native Eucalypt forest, suggesting that the Eucalypts were the strongest source of condensable vapours. Average cluster ion (0.34 to 1.8 nm) concentrations were very high, 2400/1700 cm−3 for negative/positive ions compared to other measurements around the world. These high concentrations are probably the result of the strong radon efflux from the soils around the Tumbarumba field site. Furthermore, comparison between nighttime and daytime concentrations supported the view that cluster ions are produced close to the surface within the boundary layer also at night but that large ions are mostly produced in daytime. Finally, a previously unreported phenomenon, nocturnal aerosol formation, appeared on 32% of the analysed nights but was clustered almost entirely within six months from summer to autumn in 2006. From January to May, nocturnal formation was 2.5 times as frequent as daytime formation. Therefore, it appears that in summer and autumn, nocturnal production was the major mechanism for aerosol formation in Tumbarumba.

International audience; We have measured the size distributions of air ions (0.42?7.5 nm in diameter) with the Balanced Scanning Mobility Analyzer in boreal forest, in Southern Finland since spring 2003. The size range covers the size range of cluster ions (approximately 0.42?1.6 nm) and naturally charged nanometre aerosol particles (1.6?7.5 nm) or intermediate air ions. Based on the measurements from April 2003 to March 2006 we studied the characteristics of charged aerosol particle formation by classifying each day either as a particle formation event, undefined or non-event day. The principal of the classification, as well as the statistical description of the charged aerosol particle formation events are given. We found in total 270 (26% of the analysed days) and 226 (22% of the analysed days) particle formation days for negative and positive intermediate ions, respectively. For negatively charged particles we classified 411 (40% of the analysed days) undefined and 348 (34% of the analysed days) non-event days whereas for positively charged particles 343 (33% of the analysed days) undefined and 460 (45% of the analysed days) non-event days. The results were compared with the ordinary classification based on the Differential Mobility Particle Sizer (DMPS) measurements carried out at the same place. The above-presented values differed slightly from that found from the DMPS data, with a lower particle diameter of 3 nm. In addition, we have found the rain-induced intermediate ion bursts frequently. The rain effect was detected on 163 days by means of negative ions and on 105 days by positive ones. Another interesting phenomenon among the charged aerosol particles was the appearance and existence of intermediate ions during the snowfall. We observed this phenomenon 24 times with negatively charged particles and 21 times with positively charged ones during winter months (October?April). These intermediate air ions were seen during the snowfall and may be caused by ice crystals, although the origin of these intermediate ions is unclear at the moment.

The behavior of the concentration of positive small (or cluster) air ions and naturally charged nanometer aerosol particles (aerosol ions) has been studied on the basis of measurements carried out in a boreal forest at the Hyytiälä SMEAR station, Finland, during the BIOFOR III campaign in spring 1999. Statistical characteristics of the concentrations of cluster ions, two classes of aerosol ions of the sizes of 2.5?8 nm and 8?ca. 20 nm and the quantities that determine the balance of small ions in the atmosphere have been given for the nucleation event days and non-event days. The dependence of small ion concentration on the ion loss (sink) due to aerosol particles was investigated applying a model of bipolar diffusion charging of particles by small ions. The small ion concentration and the ion sink were closely correlated (correlation coefficient ?87%) when the fog events and the hours of high relative humidity (above 95%), as well as nocturnal calms and weak wind (wind speed ?1) had been excluded. However, an extra ion loss term presumably due to small ion deposition on coniferous forest with a magnitude equal to the average ion loss to pre-existing particles is needed to explain the observations. Also the hygroscopic growth correction of measured aerosol particle size distributions was found to be necessary for proper estimation of the ion sink. In the case of nucleation burst events, variations in the concentration of small positive ions were in accordance with the changes caused by the ion sink due to aerosols; no clear indication of positive ion depletion by ion-induced nucleation was found. The estimated average ionization rate of the air at the Hyytiälä station in early spring, when the ground was partly covered with snow, was about 6 ion pairs cm?3 s?1. The study of the charging state of nanometer aerosol particles (2.5?8 nm) revealed a strong correlation (correlation coefficient 88%) between the concentrations of particles and positively charged particles (positive air ions) during nucleation bursts. The estimated charged fraction of particles, which varied from 3% to 6% considering various nucleation event days, confirms that these particles are almost quasi-steady state charged. Also the particles and air ions in the size range of 8?ca. 20 nm showed a good qualitative consistency; the correlation coefficient was 92%.

International audience; A new mathematical model describing air ion balance was developed and tested. It has improved approximations and includes dry deposition of ions onto the forest canopy. The model leads to an explicit algebraic solution of the balance equations. This allows simple calculation of both the ionization rate and the average charge of aerosol particles from measurements of air ions and aerosol particles, with some parameters of the forest. Charged aerosol particles are distinguished from cluster ions by their size, which exceeds 1.6 nm diameter. The relative uncertainty of the ionization rate is about the same or less than the relative uncertainties of the measurements. The model was tested with specific air ion measurements carried out simultaneously at two heights at the Hyytiälä forest station, Finland. Earlier studies have shown a difference in the predictions of the ionization rate in the Hyytiälä forest when calculated in two different ways: based on the measurements of the environmental radioactivity and based on the air ion and aerosol measurements. The new model explains the difference as a consequence of neglecting dry deposition of ions in the earlier models. The ionization rate during the 16 h campaign was 5.6±0.8 cm?3 s?1 at the height of 2 m and 3.9±0.2 cm?3 s?1 at the height of 14 m, between the tops of the trees. The difference points out the necessity to consider the height variation when the ionization rate is used as a parameter in studies of ion-induced nucleation. Additional results are some estimates of the parameters of air ion balance. The recombination sink of cluster ions on the ions of opposite polarity made up 9?13%, the sink on aerosol particles 65?69%, and the sink on forest canopy 18?26% of the total sink of cluster ions. The average lifetime of cluster ions was about 130 s for positive and about 110 s for negative ions. At the height of 2 m, about 70% of the space charge of air was carried by aerosol particles, and at the height of 14 m, about 84%.