Aerosol-Cloud Interaction Determined by Both in Situ and Satellite Data Over a Northern High-Latitude Site

The first aerosol indirect effect over a clean, northern high-latitude site was investigated by determining the aerosol cloud interaction (ACI) using three different approaches; ground-based in situ measurements, combined ground-based in situ measurements 5 and satellite retrievals and using only satellite retrievals. The obtained values of ACI were highest for in situ ground-based data, clearly lower for combined ground-based and satellite data, and lowest for data relying solely on satellite retrievals. One of the key findings of this study was the high sensitivity of ACI to the definition of the aerosol burden. We showed that at least a part of the variability in ACI can be explained by 10 how different investigators have related dierent cloud properties to "aerosol burden"

Growth of sulphuric acid nanoparticles under wet and dry conditions

New particle formation, which greatly influences the number concentrations and size distributions of an atmospheric aerosol, is often followed by a rapid growth of freshly formed particles. The initial growth of newly formed aerosol is the crucial process determining the fraction of nucleated particles growing to cloud condensation nuclei sizes, which have a significant influence on climate. In this study, we report the laboratory observations of the growth of nanoparticles produced by nucleation of H₂SO₄ and water in a laminar flow tube at temperatures of 283, 293 and 303 K, under dry (a relative humidity of 1%) and wet conditions (relative humidity of 30%) and residence times of 30, 45, 60 and 90 s. The initial H₂SO₄ concentration spans the range from 2 × 10⁸ to 1.4 × 10¹⁰ molecule cm⁻³ and the calculated wall losses of H₂SO₄ were assumed to be diffusion limited. The detected particle number concentrations, measured by the Ultrafine Condensation Particle Counter (UCPC) and Differential Mobility Particle Sizer (DMPS), were found to depend strongly on the residence time. Hygroscopic particle growth, presented by growth factors, was found to be in good agreement with the previously reported studies. The experimental growth rates ranged from 20 nm h⁻¹ to 890 nm h⁻¹ at relative humidity (RH) 1% and from 7 nm h⁻¹ to 980 nm h⁻¹ at RH 30% and were found to increase significantly with the increasing concentration of H₂SO₄. Increases in the nucleation temperature had a slight enhancing effect on the growth rates under dry conditions. The influence of relative humidity on growth was not consistent – at lower H₂SO₄ concentrations, the growth rates were higher under dry conditions while at H₂SO₄ concentrations greater than 1 × 10¹⁰ molecule cm⁻³, the growth rates were higher under wet conditions. The growth rates show only a weak dependence on the residence time. The experimental observations were compared with predictions made using a numerical model, which investigates the growth of particles with three different extents of neutralization by ammonia, NH₃: (1) pure H₂SO₄ – H₂O particles; (2) particles formed by ammonium bisulphate, (NH₄)HSO₄; (3) particles formed by ammonium sulphate, (NH₄)₂SO₄. The highest growth rates were found for ammonium sulphate particles. Since the model accounting for the initial H₂SO₄ concentration predicted the experimental growth rates correctly, our results suggest that the commonly presumed diffusional wall losses of H₂SO₄ in case of long-lasting experiments are not so significant. We therefore assume that there are not only losses of H₂SO₄ on the wall, but also a flux of H₂SO₄ molecules from the wall into the flow tube, the effect being more profound under dry conditions and at higher temperatures of the tube wall. Based on a comparison with the atmospheric observations, our results indicate that sulphuric acid alone cannot explain the growth rates of particles formed in the atmosphere

Deterioration of air quality across Sweden due to transboundary agricultural burning emissions

Targino, A. C., Krecl, P., Johansson, C., Swietlicki, E., Massling, A., Coraiola, G. C. & Lihavainen, H. 2013: Deterioration of air quality across Sweden due to transboundary agricultural burning emissions. Boreal Env. Res. 18: 19-36. We analyzed measurements of aerosol and trace-gas concentrations from sites across Sweden before and during a series of agricultural wildland fires in eastern Europe in spring 2006. During the burning episodes, concentrations of background particulate matter (PM) and trace gases, such as carbon monoxide and ozone, increased, affecting air quality across the country and violating national air quality standards. The European Union PM10 daily limit value of 50 mu g m(-3) was exceeded during the pollution episodes even at the background stations, resulting in a nearly four-fold increase as compared with that in non-episode conditions. In relation to a non-episode period, the concentration rise in the accumulation-mode particles was from 40% at an urban site to 340% at a rural site, causing an increase in total particle number concentrations. The fires also boosted ground-level ozone, increasing concentrations of this pollutant by up to 100% at the background stations, which exceeded national air quality standards. Both elemental (EC) and organic carbon (OC) levels increased, with OC making a larger contribution to the total carbonaceous concentrations during the biomass burning episodes. The large-scale atmospheric circulation determined the strength and timing of the pollution events, with the eastern and northern sectors of Sweden experiencing two pollution pulses, whilst sites in the western and southern sectors were affected by one shorter episode. The results show that regional air quality deteriorated due to the long-range transport of pollutants emitted during agricultural wildfires

Mobile Aerosol Measurement in the Eastern Mediterranean – A Utilization of Portable Instruments

Air pollution research and reports have been limited in the Middle East, especially in Jordan with respect to aerosol particle number concentrations. In this study, we utilized a simple "mobile setup" to measure, for the first time, the spatial variation of aerosol concentrations in Eastern Mediterranean. The mobile setup consisted of portable aerosol instruments to measure particle number concentrations (cut off sizes 0.01, 0.02, 0.3, 0.5, 1, 2.5, 5, and 10 mu m), particle mass concentrations (PM1, PM2.5, and PM10), and black carbon concentration all situated on the back seat of a sedan car. The car was driven with open windows to ensure sufficient cabin air ventilation for reliable outdoor aerosol sampling. Although the measurement campaign was two days long, but it provided preliminary information about aerosols concentrations over a large spatial scale that covered more than three quarters of Jordan. We should keep in mind that the presented concentrations reflect on road conditions. The submicron particle concentrations were the highest in the urban locations (e.g., Amman and Zarqa) and inside cities with heavy duty vehicles activities (e.g., Azraq). The highest micron particle concentrations were observed in the southern part of the country and in places close to the desert area (e.g., Wadi Rum and Wadi Araba). The average submicron concentration was 4.9 x 10(3)-120 x 10(3) cm-3 (5.7-86.7 mu g m(-3)) whereas the average micron particle concentration was 1-11 cm(-3) (8-150 mu g m(-3), assume rho(p) = 1 g cm(-3)). The main road passing through Jafr in the eastern part of Jordan exhibited submicron concentration as low as 800 cm(-3). The PM10 concentration consisted of about 40-75% as PM1. The black carbon (BC) concentration variation was in good agreement with the PM1 as well as the submicron particle number concentration.Peer reviewe

Boundary layer concentrations and landscape scale emissions of volatile organic compounds in early spring

International audienceBoundary layer concentrations of several volatile organic compounds (VOC) were measured during two campaigns in springs of 2003 and 2006. The measurements were conducted over boreal landscapes near SMEAR II measurement station in Hyytiälä, Southern Finland. In 2003 the measuremens were performed using a light aircraft and in 2006 using a hot air balloon. Isoprene concentrations were low, usually below detection limit. This can be explained by low biogenic production due to cold weather, phenological stage of the isoprene emitting plants, and snow cover. Monoterpenes were observed frequently. The average total monoterpene concentration in the boundary layer was 33 pptv. Many anthropogenic compounds such as benzene, xylene and toluene, were observed in high amounts. Ecosystem scale surface emissions were estimated using a simple mixed box budget methodology. Total monoterpene emissions varied up to 80 ?g m?2 h?1, ?-pinene contributing typically more than two thirds of that. These emissions were somewhat higher that those calculated using emission algorithm. The highest emissions of anthropogenic compounds were those of p/m xylene

Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

We use observations of total particle number concentration at 36 worldwide sites and a global aerosol model to quantify the primary and secondary sources of particle number. We show that emissions of primary particles can reasonably reproduce the spatial pattern of observed condensation nuclei (CN) (R2=0.51) but fail to explain the observed seasonal cycle at many sites (R2=0.1). The modeled CN concentration in the free troposphere is biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles is included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental boundary layer (BL) are also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles is increased or an empirical BL particle formation mechanism based on sulfuric acid is used. We find that the seasonal CN cycle observed at continental BL sites is better simulated by including a BL particle formation mechanism (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). Using sensitivity tests we derive optimum rate coefficients for this nucleation mechanism, which agree with values derived from detailed case studies at individual sites

Measurements of optical properties of atmospheric aerosols in Northern Finland

International audienceThree years of continuous measurements of aerosol optical properties and simultaneous aerosol number size distribution measurements at Pallas GAW station, a remote subarctic site in the northern border of the boreal forest zone, have been analysed. The scattering coefficient at 550 nm varied from 0.2 to 94.4 Mm?1 with an average of 7.1±8.6 Mm?1. Both the scattering and backscattering coefficients had a clear seasonal cycle with an autumn minimum and a 4?5 times higher summer maximum. The scattering was dominated by submicron aerosols and especially so during late summer and autumn. The Ångström exponent had a clear seasonal pattern with maximum values in late summer and minimum values during wintertime. The highest hemispheric backscattering fraction values were observed in autumn, indicating clean air with few scattering particles and a particle size distribution strongly dominated by ultrafine particles. To analyse the influence of air mass origin on the aerosol optical properties a trajectory climatology was applied to the Pallas aerosol data. The most polluted trajectory patterns represented air masses from the Kola Peninsula, Scandinavia and Russia as well as long-range transport from Britain and Eastern Europe. These air masses had the largest average scattering and backscattering coefficients for all seasons. Higher than average values of the Ångström exponent were also observed in connection with transport from these areas

Evaluating the Assumptions of Surface Reflectance and Aerosol Type Selection Within the MODIS Aerosol Retrieval Over Land: The Problem of Dust Type Selection

Aerosol Optical Depth (AOD) and Angstrom exponent (AE) values derived with the MODIS retrieval algorithm over land (Collection 5) are compared with ground based sun photometer measurements at eleven sites spanning the globe. Although, in general, total AOD compares well at these sites (R2 values generally over 0.8), there are cases (from 2 to 67% of the measurements depending on the site) where MODIS clearly retrieves the wrong spectral dependence, and hence, an unrealistic AE value. Some of these poor AE retrievals are due to the aerosol signal being too small (total AOD<0.3) but in other cases the AOD should have been high enough to derive accurate AE. However, in these cases, MODIS indicates AE values close to 0.6 and zero fine model weighting (FMW), i.e. dust model provides the best fitting to the MODIS observed reflectance. Yet, according to evidence from the collocated sun photometer measurements and back-trajectory analyses, there should be no dust present. This indicates that the assumptions about aerosol model and surface properties made by the MODIS algorithm may have been incorrect. Here we focus on problems related to parameterization of the land-surface optical properties in the algorithm, in particular the relationship between the surface reflectance at 660 and 2130 nm

Airborne measurements of nucleation mode particles I: coastal nucleation and growth rates

International audienceA light aircraft was equipped with a bank of Condensation Particle Counters (CPCs) (50% cut from 3?5.4?9.6 nm) and a nano-Scanning Mobility Particle Sizer (nSMPS) and deployed along the west coast of Ireland, in the vicinity of Mace Head. The objective of the exercise was to provide high resolution micro-physical measurements of the coastal nucleation mode in order to map the spatial extent of new particle production regions and to evaluate the evolution, and associated growth rates of the coastal nucleation-mode aerosol plume. Results indicate that coastal new particle production is occurring over most areas along the land-sea interface with peak concentrations at the coastal plume-head in excess of 106 cm?3. Pseudo-Lagrangian studies of the coastal plume evolution illustrated significant growth of new particles to sizes in excess of 8 nm approximately 10 km downwind of the source region. Close to the plume head (?1, decreasing gradually to 53?72 nm h?1 at 3 km. Further along the plume, at distances up to 10 km, the growth rates are calculated to be 17?32 nm h?1. Growth rates of this magnitude suggest that after a couple of hours, coastal nucleation mode particles can reach significant sizes where they can contribution to the regional aerosol loading