Chemical characterization of non-refractory submicron particles (NR-PM1) and source apportionment of organic aerosols (OA) were carried out at four different sites in the Helsinki metropolitan area, Finland, using an Aerodyne Aerosol Chemical Speciation Monitor (ACSM). Two of the sites represented suburban residential areas, whereas the other two were traffic sites, one in a curbside in downtown and the other one in a suburban highway edge. The residential and the curbside measurements were conducted during the winter, but the highway campaign was carried out in the autumn. NR-PM1 were composed mainly of organics (40–68

A two weeks measurement campaign by a mobile laboratory van was performed at downtown Helsinki, Finland, in winter 2010. The characteristics of air pollutants such as fine particles in the size ranges of 7–40 nm (Np40) and 40–1000 nm (Np1000), black carbon (BC), fine particle mass (PM2.5), as well as gaseous compounds NO, NO2, NOx, CO and CO2 were studied. The statistical analysis showed that the air pollution conditions strongly depended on the traffic flow area; therefore, the street sections were classified as high traffic flow areas (HTF1-HTF4), low traffic flow areas (LTF1-LTF5), and urban background areas (BG1-BG3). Large variation of particle emissions was observed, and the momentary peak particle concentrations were 8 × 105 cm–3. At the HTF areas exhaust emissions followed clearly daily average heavy duty vehicle counts rather than the average daily vehicle counts. Higher correlation coefficients were found between CO2 and NO than between CO2 and Ntot. The dispersion studies indicated that the air pollution conditions strongly improved from high traffic flow areas to low traffic flow areas. Therefore, proper city planning and locating, for example, cycle tracks, schools and hospitals farther from busy city streets might significantly reduce exposure risk for humans.

High time resolution chemical characterization of submicron particles was carried out in the South American city of Santiago de Chile using the Aerosol Chemical Speciation Monitor (ACSM). The instrumentation operated for 100 days from August 17th to November 23rd 2011 in an urban station located inside the University of Santiago de Chile (USACH) campus. In addition, a semi-continuous OC/EC analyzer was also run in parallel with the ACSM for some of this time. Meteorological conditions varied along the studied period due to the transition from winter to spring time. Atmospheric temperature inversions were responsible for hourly average sub-micron particulate matter levels of up to 80 μg/m3, especially during the night time. The average submicron particle mass concentration (± standard deviation) for the whole period was 29.8 ± 25 μg/m3. Aerosol particles were composed mainly of organics 59

Climate services are becoming the backbone to translate climate knowledge, data & information into climate-informed decision-making at all levels, from public administrations to business operators. It is essential to assess the technical and scientific quality of the provided climate data and information products, including their value to users, to establish the relation of trust between providers of climate data and information and various downstream users. The climate data and information products (i.e., from satellite, in-situ and reanalysis) shall be fully traceable, adequately documented and uncertainty quantified and can provide sufficient guidance for users to address their specific needs and feedbacks. This paper discusses details on how to apply the quality assurance framework to deliver timely assessments of the quality and usability of Essential Climate Variable (ECV) products. It identifies an overarching structure for the quality assessment of single product ECVs (i.e., consists of only one single variable), multi-product ECVs (i.e., more than one single parameter), thematic products (i.e., water, energy and carbon cycles), as well as the usability assessment. To support a traceable climate service, other than rigorously evaluating the technical and scientific quality of ECV products, which represent the upstream of climate services, how the uncertainty propagates into the resulting benefit (utility) for the users of the climate service needs to be detailed.

Aerosol chemical and physical properties were measured in 2010 at Neumayer research station, Antarctica. Samples for chemical analysis (ion chromatography) were collected using a Teflon/Nylon filter combination (Thy) sampler, and with a multi stage low pressure impactor (SDI). Particle number concentration was measured continuously with a Grimm OPC optical particle counter. Total particle number concentration varied largely throughout the year, and the highest number concentrations for particles larger than 0.3 mu m were observed simultaneously with the highest sea salt concentrations. About 50% of the sea salt aerosol mass was found in the submicron size range. Below 0.2 mu m of particle aerodynamic diameter the contribution of sea salt aerosols was negligible. Further analysis showed that sea salt aerosols had undergone physico-chemical processes, either during the transportation, or during their formation. High degree of chloride depletion was observed during austral summer, when the presence of acidic gases exhibit their characteristic seasonal maximum. Apart from chloride depletion, excess chloride relating to sodium was also detected in one SDI sample, indicating actually a sodium depletion by mirabilite formation on freshly formed sea ice areas. Analysis of selected episodes showed that the concentration of sea salt particles, their modal structure, and their chemical composition is connected with their source areas, their formation mechanisms, and local transport history. (C) 2014 Published by Elsevier Ltd.

Globally more than a quarter of the total primary energy supply is based on coal combustion. The emissions of coal-fired power plants (CFPPs) are regulated in many industrialized countries and therefore power plants use cleaning techniques to minimize emissions such as sulfur dioxide (SO2) and particles. In this study, the particulate emissions from coal combustion were investigated at a CFPP (506MW) used for combined heat and power production in Helsinki, Finland. Fine particle samples (PM1) were collected after electrostatic precipitator before the desulfurization plant (DSP), including flue gas desulfurization unit (FGD) and baghouse filters, and simultaneously in the smokestack to study the influence of DSP to particulate mass and chemistry. The DSP removed over 97% of particle mass in flue gas. Trace metals were removed efficiently but contribution of some ionic compounds increased in the FGD process. The particle properties were studied in more detail in the smokestack including particle size distribution measurements and size-segregating sampling to study chemical composition and morphology of particles. The particulate emissions from the CFPP were relatively small, consisting mainly of products and reagents of the FGD process (e.g., CaSO4, NaCl) and partly of the primary emissions from the coal combustion (e.g., mineral ash and reaction products of gas phase components). The maximum in particle volume was detected at 0.68µm. PM1 contributed on average 62 ± 5% to PM10 mass. Besides particulate matter, also the gas-phase emission of mercury was studied because coal combustion is one of the major sources of mercury found in the environment. The mercury emissions were within the proposed limits in the EU.

Particle emissions affect radiative forcing in the atmosphere. Therefore, it is essential to know the physical and chemical characteristics of them. This work studied the chemical, physical, and optical characteristics of particle emissions from small-scale wood combustion, coal combustion of a heating and power plant, as well as heavy and light fuel oil combustion at a district heating station. Fine particle (PM1) emissions were the highest in wood combustion with a high fraction of absorbing material. The emissions were lowest from coal combustion mostly because of efficient cleaning techniques used at the power plant. The chemical composition of aerosols from coal and oil combustion included mostly ions and trace elements with a rather low fraction of absorbing material. The single scattering albedo and aerosol forcing efficiency showed that primary particles emitted from wood combustion and some cases of oil combustion would have a clear climate warming effect even over dark earth surfaces. Instead, coal combustion particle emissions had a cooling effect. Secondary processes in the atmosphere will further change the radiative properties of these emissions but are not considered in this study.

Concentration and composition of the fine particulate matter (PM) was measured using various online methods for 13 months in an urban, background area in Helsinki, Finland. Seasonal differences were found for ions and carbonaceous compounds. Biomass burning was found to increase inorganic ion and elemental carbon (EC) concentrations in winter, whereas organic carbon (OC) contribution was highest during summer due to secondary aerosol formation. Diurnal cycles, with maxima between 06:00 and 09:00, were recorded for EC and nitrate due to traffic emissions. In addition, the concentrations measured with the online and offline PM sampling devices were compared using regression analysis. In general, a good agreement (r(2) = 0.60-0.95) was found. During the year-long measurements, on average 65% of PM2.5 was identified by submicron chemical analyses (ions, OC, EC). As compared with filter measurements, the high resolution measurements provided important data on short pollution plumes and diurnal changes.

Heavy fuel oil (HFO) is a commonly used fuel in industrial heating and power generation and for large marine vessels. In this study, the fine particle emissions of a 47 MW oil-fired boiler were studied at 30 MW power and with three different fuels. The studied fuels were HFO, water emulsion of HFO, and water emulsion of HFO mixed with light fuel oil (LFO). With all the fuels, the boiler emitted considerable amounts of particles smaller than 200 nm in diameter. Further, these small particles were quite hygroscopic even as fresh and, in the case of HFO+LFO emulsion, the hygroscopic growth of the particles was dependent on particle size. The use of emulsions and the addition of LFO to the fuel had a reducing effect on the hygroscopic growth of particles. The use of emulsions lowered the sulfate content of the smallest particles but did not affect significantly the sulfate content of particles larger than 42 nm and, further, the addition of LFO considerably increased the black carbon content of particulate matter. The results indicate that even the fine particles emitted from HFO based combustion can have a significant effect on cloud formation, visibility, and air quality.

Measurements of submicron particulate matter (PM) were performed at an urban background station, in Helsinki, Finland during wintertime to investigate the chemical characteristics and sources of PM1. The PM1 was dominated by sulfate and organics. The source apportionment indicated that organic aerosol (OA) was a mixture from local sources (biomass burning (BBOA), traffic, coffee roaster (CROA)), secondary compounds formed in local wintertime conditions (nitrogen containing OA (NOA), semivolatile oxygenated OA (SV-OOA), and regional and long-range transported compounds (low volatile oxygenated OA, LV-OOA). BBOA was dominated by the fragments C2H4O2 + and C3H4O2 + (m/z 60.021 and 73.029) from levoglucosan, or other similar sugar components, comprising on average 32% of the BBOA mass concentration. The ratio between fragments C2H4O2 +/C3H4O2 + was significantly lower for CROA (=1.1) when compared to BBOA (=2.1), indicating that they consisted of different sugar compounds. In addition, a component containing substantial amount of nitrogen compounds (NOA) was observed in a sub-arctic region for the first time. The NOA contribution to OA ranged from 1% to 29% and elevated concentrations were observed when ambient relative humidity was high and the visibility low. Low solar radiation and temperature in wintertime were observed to influence the oxidation of compounds. A change in aerosol composition, with an increase of LV-OOA and decrease in BBOA, SV-OOA and NOA was noticed during the transition from wintertime to springtime. Size distribution measurements with high-time resolution enabled chemical characterization of externally mixed aerosol from different sources. Aged regional long-range transported aerosols were dominant at around 0.5 μm (vacuum aerodynamic diameter), whereas traffic and CROA emissions dominated at around 120 nm. Copyright 2014 American Association for Aerosol Research

Heavy fuel oil (HFO) is used widely in industrial scale energy production (heat and power), and in large marine vessels. HFO includes many impurities which affect the particle emissions and, further, the air quality and human exposure on particles. Depending on characteristics of particles, the particle emissions from combustion of HFO may affect also the climate. The primary particulate matter emitted in HFO combustion has been known to contain metallic and sulphur compounds. The combustion of HFO is known to produce also considerable amounts of sulphur oxides which can contribute to the particulate formation in the atmosphere. In order to decrease the high PM and sulphur emissions of HFO combustion, the knowledge related to particle characteristics and formation as well as to the effects of fuel composition and flue gas cleaning on the particles is needed. In this study we focused on the detailed characterization of particles emitted from an HFO-fired boiler having nominal power of 47 MW. The measurements were performed at 30 MW power and with three different fuels. The studied fuels were HFO, water emulsion of HFO and water emulsion of HFO mixed with light fuel oil (LFO). The flue gas was sampled continuously by using a Fine Particle Sampler (FPS, Dekati Inc.). After that, the number size distribution, volatility and hygroscopicity of particles were studied. Particle number size distributions were studied using two scanning mobility particle sizers (SMPS, TSI Inc.) and an electrical low pressure impactor (ELPI, Dekati Inc.). In the hygroscopicity studies we used a hygroscopic tandem differential mobility analyzer (HTDMA). The particle volatility was studied by treating the diluted flue gas sample with a thermodenuder and, after that, by measuring the effects of the treatment on the particle size distribution and hygroscopicity. In addition, these studies were supported by comprehensive analyses for particle chemical composition. For more detailed description of the measurements, see Happonen et al. (2013). With all the studied fuels, the particle number size distribution was dominated by particles smaller than 100 nm in diameter. These small particles were observed to consist mainly of nonvolatile compounds. The particles were observed to be quite hygroscopic even as fresh. In addition, especially when the fuel was water emulsion of the mixture of HFO and LFO, the hygroscopicity of the particles was strongly dependent on particle size; the hygroscopicity of larger particles was observed to be significantly lower than the hygroscopicity of smaller particles. In general, the results indicate that even the fine particles emitted from HFO based combustion can have a significant effect on cloud formation, visibility and air quality. The research was part of the Measurement, Monitoring and Environmental Assessment (MMEA) program. References: Happonen, M., et al. 2013. Size distribution, chemical composition, and hygroscopicity of fine particles emitted from an oil-fired heating plant. Environmental Science & Technology, DOI: 10.1021/es4028056.

Department of Technology, Metropolia University of Applied Sciences, P.O. Box 4021, FI-00180 Helsinki, Finland Department of Physics, University of Helsinki, P.O. Box 64, FI-00014 Helsinki, Finland Helsinki Region Environmental Services Authority HSY, P.O. Box 100, FI-00066 HSY, Finland Aerosol Physics Laboratory, Tampere University of Technology, P.O. Box 527, FI-33101 Tampere, Finland Finnish Meteorological Institute, P.O. Box 503, FI-00101 Helsinki, Finland

A measurement campaign by a mobile laboratory van was performed in urban microenvironments bounded by a busy street Mannerheimintie in the city center of Helsinki, Finland. The characteristics of spatiotemporally high-resolution pollutant concentrations were studied such as ultrafine particles in the size range of 3-414 nm, black carbon BC, fine particle mass PM2.5, as well as nitrogen oxides NO and NO2. In addition, the effects of street geometry and roadside structure on the local dispersion of traffic emissions were analyzed as well. Meteorological conditions stayed stable and the wind direction was perpendicular to Mannerheimintie during the campaign. The highest particle concentrations were similar to 8 x 10(5) cm(-3), of which around 94% was smaller than 40 nm. At the pavement, the average concentration was in maximum 5 x 10(4) cm(-3); around 80% of the particles was smaller than 40 nm. The volatility fraction was 75% by number. Due to the street canyon effect by the surrounding buildings, the downwind concentrations were around 24% of the upwind concentrations for particle number, 28% of NO, 39% of BC and 70% of NO2 concentrations. Furthermore, the upwind concentrations were higher than the simultaneously measured concentrations within the traffic flow. In fact, the particle count was around 3-fold, BC 2.5-fold, PM2.5 and NO2 1.5-fold compared to the concentrations while driving. Thus, for this measurement site and under these meteorological conditions, the exposure to pedestrians and cyclist on the upwind pavement is even higher than the driver's exposure. If the downwind buildings were parallel to Mannerheimintie, the concentrations dropped significantly at the pavement and continued decreasing slightly in the courtyards. When the downwind buildings were perpendicular to Mannerheimintie, a gradual reduction in the concentrations between the buildings was observed. However, at a distance of approximately a hundred meters a parallel side street which was a street canyon, started to affect the concentrations resulting in an increased exposure risk for pedestrians and cyclists. Understanding the local transport and the dispersion of traffic emissions are important for city planning and air quality assessment. (C) 2012 Elsevier Ltd. All rights reserved.

Abstract. Year-long high timeresolution measurements of major chemical components in atmospheric sub-micrometer particles were conducted at an urban background station in Finland 2006–2007. Ions were analyzed using a particle-into-liquid sampler combined with an ion chromatograph (PILS-IC), organic and elemental carbon (OC and EC) by using a semicontinuos OC/EC aerosol carbon analyzer (RT-OCEC), and PM2.5 mass with a tapered element oscillating microbalance (TEOM). Long time series provides information on differences between the used measurement techniques as well as information about the diurnal and seasonal changes. Chemical mass closure was constructed by comparing the identified aerosol mass with the measured PM2.5. The sum of all components measured online (ions, particulate organic matter (POM), EC) represented only 65% of the total PM2.5 mass. The difference can be explained by the difference in cutoff sizes (PM1 for online measurements, PM2.5 for total mass) and by evaporation of the semivolatile/volatile components. In general, some differences in results were observed when the results of the continuous/semicontinuous instruments were compared with those of the conventional filter samplings. For non-volatile compounds, like sulfate and potassium, correlation between the filter samples and the PILS was good but greater differences were observed for the semivolatile compounds like nitrate and ammonium. For OC the results of the RT-OCEC were on average 10% larger than those of the filters. When compared to filter measurements, high resolution measurements provide important data on short pollution plumes as well as on diurnal changes. Clear seasonal and diurnal cycles were observed for nitrate and EC.

The volcanic eruption of Grimsvötn in Iceland in May 2011 affected surface-layer air quality at several locations in Northern Europe. In Helsinki, Finland, the main pollution episode lasted for more than 8 h around the noon of 25 May. We characterized this episode by relying on detailed physical, chemical and optical aerosol measurements. The analysis was aided by air mass trajectory calculations, satellite measurements, and dispersion model simulations. During the episode, volcanic ash particles were present at sizes from less than 0.5 μm up to sizes >10 μm. The mass mean diameter of ash particles was a few μm in the Helsinki area, and the ash enhanced PM10 mass concentrations up to several tens of μg m−3. Individual particle analysis showed that some ash particles appeared almost non-reacted during the atmospheric transportation, while most of them were mixed with sea salt or other type of particulate matter. Also sulfate of volcanic origin appeared to have been transported to our measurement site, but its contribution to the aerosol mass was minor due the separation of ash-particle and sulfur dioxide plumes shortly after the eruption. The volcanic material had very little effect on PM1 mass concentrations or sub-micron particle number size distributions in the Helsinki area. The aerosol scattering coefficient was increased and visibility was slightly decreased during the episode, but in general changes in aerosol optical properties due to volcanic aerosols seem to be difficult to be distinguished from those induced by other pollutants present in a continental boundary layer. The case investigated here demonstrates clearly the power of combining surface aerosol measurements, dispersion model simulations and satellite measurements in analyzing surface air pollution episodes caused by volcanic eruptions. None of these three approaches alone would be sufficient to forecast, or even to unambiguously identify, such episodes.

Abstract. Light absorption measurements most commonly rely on filter-based measurement techniques. These methods are disturbed by light scattering constituents in the aerosol phase deposited on the filters. The light scattering material changes the optical path of light in the filter matrix increasing the light absorption of the filter. Measurement equipment interpret this wrongly as light absorption by the aerosol. Most light scattering constituents in a sub-micron aerosol are volatile by their nature and they can be volatilized by heating the sample air. This volatilisation significantly alters the optical properties of the urban aerosol and was studied during a short field campaign with two groups of equipment measuring in parallel for six days in April 2009 at the SMEAR III station in Helsinki. When heated, the light scattering constituents were evaporated thus reducing the single-scattering albedo (ω0) of the aerosol by as much as 0.4. With less light scattering constituents in the aerosol phase the mass absorption cross section (MAC) of soot was calculated to be 13.5±0.5 m2 g−1 at λ=545 nm. An oven was set to scan different temperatures which revealed the volatility of the urban aerosol at different temperatures as well as the single-scattering albedo's dependence on the non-volatile volume fraction remaining (NVFR). At 50 °C 79±13% of the volume remained while only 46±8% remained at 150 °C and just 23±6% at 280 °C. At 50 °C ω0 was 0.65±0.06, at 150 °C ω0=0.54±0.06 and at 280 °C ω0=0.33±0.06. We found that absorption coefficients measured at different temperatures showed a temperature dependency possibly indicating initially different mixing states of the non-volatile constituents.

Residential heating is an important local source of fine particles and may cause significant exposure and health effects in populations. We investigated the cytotoxic and inflammatory activity of particulate emissions from normal (NC) and smouldering (SC) combustion in one masonry heater. The PM1-0.2 and PM0.2 samples were collected from the dilution tunnel with a high-volume cascade impactor (HVCI). Mouse RAW 264.7 macrophages were exposed to the PM-samples for 24 h. Inflammatory mediators, (IL-6, TNF alpha and MIP-2), and cytotoxicity (MTT-test), were measured. Furthermore, apoptosis and cell cycle of macrophages were analyzed. The HVCI particulate samples were characterized for ions, elements and PAH compounds. Assays of elemental and organic carbon were conducted from parallel low volume samples. All the samples displayed mostly dose-dependent inflammatory and cytotoxic activity. SC samples were more potent than NC samples at inducing cytotoxicity and MIP-2 production, while the order of potency was reversed in TNF alpha production. SC-PM1-0.2 sample was a significantly more potent inducer of apoptosis than the respective NC sample. After adjustment for the relative toxicity with emission factor (mg MJ(-1)), the SC-PM emissions had clearly higher inflammatory and cytotoxic potential than the NC-PM emissions. Thus, operational practice in batch burning of wood and the resultant combustion condition clearly affect the toxic potential of particulate emissions. (C) 2010 Elsevier Ltd. All rights reserved.

Aerosol light absorption measurements most commonly rely on filter-based techniques. These methods are influenced by light scattering constituents in the aerosol phase deposited on the filters. The coating of soot by non-absorbing constituents changes the mixing state of soot as the aerosol ages and increase light absorption by the aerosol. Most light scattering constituents in a sub-micron aerosol are volatile by their nature due to their chemical composition and can be volatilized by heating the sample air. The initial mixing state is lost but the remaining light absorption by the aerosol should be by non-coated soot alone.This was studied during a short field campaign with two groups of equipment measuring in parallel for six days in April 2009 at the SMEAR III station in Helsinki. When heated, the light scattering constituents were evaporated thus reducing the single-scattering albedo (ω0) of the aerosol by as much as 0.4. An oven was set to scan different temperatures which revealed the volatility of the urban aerosol at different temperatures as well as the single-scattering albedo's dependence on the non-volatile volume fraction remaining (NVFR). The NVFR was 0.72 ± 0.13, 0.42 ± 0.06 and 0.22 ± 0.05 at 50, 150 and 280 °C respectively. ω0 behaved analogically, it was 0.71 ± 0.05, 0.62 ± 0.06 and 0.42 ± 0.07 at the respective temperatures. We found that absorption coefficients measured at different temperatures showed a temperature dependency possibly indicating initially different mixing states of the non-volatile constituents.By heating the aerosol the mode of the size distribution gets shifted to smaller sizes which in turn changes the filter-based instrument's response due increased penetration depth into the filter by the smaller residual particles. This was compensated for by using size distribution data.

Abstract. The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm) and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.