Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä

This study investigates the connections between atmospheric sulphuric acid and new particle formation during QUEST III and BACCI/QUEST IV campaigns. The campaigns have been conducted in Heidelberg (2004) and Hyytiälä (2005), the first representing a polluted site surrounded by deciduous forest, and the second a rural site in a boreal forest environment. We have studied the role of sulphuric acid in particle formation and growth by determining 1) the power-law dependencies between sulphuric acid ([H2SO4]), and particle concentrations (N3−6) or formation rates at 1 nm and 3 nm (J1 and J3); 2) the time delays between [H2SO4] and N3−6 or J3, and the growth rates for 1–3 nm particles; 3) the empirical nucleation coefficients A and K in relations J1=A[H2SO4] and J1=K[H2SO4]^2, respectively; 4) theoretical predictions for J1 and J3 for the days when no significant particle formation is observed, based on the observed sulphuric acid concentrations and condensation sinks. In both environments, N3−6 or J3 and [H2SO4] were linked via a power-law relation with exponents typically ranging from 1 to 2. The result suggests that the cluster activation theory and kinetic nucleation have the potential to explain the observed particle formation. However, some differences between the sites existed: The nucleation coefficients were about an order of magnitude greater in Heidelberg than in Hyytiälä conditions. The time lags between J3 and [H2SO4] were consistently lower than the corresponding delays between N3−6 and [H2SO4]. The exponents in the J3/[H2SO4]^n_(J3)-connection were consistently higher than or equal to the exponents in the relation N3−6/[H2SO4]^n_(N36). In the J1 values, no significant differences were found between the observed rates on particle formation event days and the predictions on non-event days. The J3 values predicted by the cluster activation or kinetic nucleation hypotheses, on the other hand, were considerably lower on non-event days than the rates observed on particle formation event days. This study provides clear evidence implying that the main process limiting the observable particle formation is the competition between the growth of the freshly formed particles and their loss by scavenging, rather than the initial particle production by nucleation of sulphuric acid. In general, it can be concluded that the simple models based on sulphuric acid concentrations and particle formation by cluster activation or kinetic nucleation can predict the occurence of atmospheric particle formation and growth well, if the particle scavenging is accurately accounted for

Chemical composition of boundary layer aerosol over the Atlantic Ocean and at an Antarctic site

International audienceAerosol chemical composition was measured over the Atlantic Ocean in November?December 1999 and at the Finnish Antarctic research station Aboa in January 2000. The concentrations of all anthropogenic aerosol compounds decreased clearly from north to south. An anthropogenic influence was still evident in the middle of the tropical South Atlantic, background values were reached south of Cape Town. Chemical mass balance was calculated for high volume filter samples (Dp80% in the Southern Ocean, and 10% in most samples, also at Aboa. The correlation of biomass-burning-related aerosol components with 210Pb was very high compared with that between nss calcium and 210Pb which suggests that 210Pb is a better tracer for biomass burning than for Saharan dust. The ratio of the two clear tracers for biomass burning, nss potassium and oxalate, was different in European and in African samples, suggesting that this ratio could be used as an indicator of biomass burning type. The concentrations of continent-related particles decreased exponentially with the distance from Africa. The shortest half-value distance, ~100 km, was for nss calcium. The half-value distance of particles that are mainly in the submicron particles was ~700±200 km. The MSA to nss sulfate ratio, R, increased faster than MSA concentration with decreasing anthropogenic influence, indicating that the R increase could largely be explained by the decrease of anthropogenic sulfate

Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä

This study investigates the connections between atmospheric sulphuric acid and new particle formation during QUEST III and BACCI/QUEST IV campaigns. The campaigns have been conducted in Heidelberg (2004) and Hyytiälä (2005), the first representing a polluted site surrounded by deciduous forest, and the second a rural site in a boreal forest environment. We have studied the role of sulphuric acid in particle formation and growth by determining 1) the power-law dependencies between sulphuric acid ([H₂SO₄]), and particle concentrations (<I>N</I>_3&ndash;6) or formation rates at 1 nm and 3 nm (<I>J</i>₁ and <I>J</I>₃); 2) the time delays between [H₂SO₄] and <I>N</I>_3&ndash;6 or <I>J</I>₃, and the growth rates for 1&ndash;3 nm particles; 3) the empirical nucleation coefficients <I>A</I> and <I>K</I> in relations <I>J</I>₁=<I>A</I>[H₂SO₄] and <I>J</I>₁=<I>K</I>[H₂SO₄]², respectively; 4) theoretical predictions for <I>J</I>₁ and <I>J</I>₃ for the days when no significant particle formation is observed, based on the observed sulphuric acid concentrations and condensation sinks. In both environments, <I>N</I>_3&ndash;6 or <I>J</I>₃ and [H₂SO₄] were linked via a power-law relation with exponents typically ranging from 1 to 2. The result suggests that the cluster activation theory and kinetic nucleation have the potential to explain the observed particle formation. However, some differences between the sites existed: The nucleation coefficients were about an order of magnitude greater in Heidelberg than in Hyytiälä conditions. The time lags between <I>J</I>₃ and [H₂SO₄] were consistently lower than the corresponding delays between <I>N</I>_3&ndash;6 and [H₂SO₄]. The exponents in the <I>J</I>₃&#x221D;[H₂SO₄ ]^n_J3-connection were consistently higher than or equal to the exponents in the relation <I>N</I>_3&ndash;6&#x221D;[H₂SO₄ ]^n_N36. In the <I>J</I>₁ values, no significant differences were found between the observed rates on particle formation event days and the predictions on non-event days. The <I>J</I>₃ values predicted by the cluster activation or kinetic nucleation hypotheses, on the other hand, were considerably lower on non-event days than the rates observed on particle formation event days. This study provides clear evidence implying that the main process limiting the observable particle formation is the competition between the growth of the freshly formed particles and their loss by scavenging, rather than the initial particle production by nucleation of sulphuric acid. In general, it can be concluded that the simple models based on sulphuric acid concentrations and particle formation by cluster activation or kinetic nucleation can predict the occurence of atmospheric particle formation and growth well, if the particle scavenging is accurately accounted for

Using a moving measurement platform for determining the chemical composition of atmospheric aerosols between Moscow and Vladivostok

The TROICA-9 expedition (Trans-Siberian Observations Into the Chemistry of the Atmosphere) was carried out at the Trans-Siberian railway between Moscow and Vladivostok in October 2005. Measurements of aerosol physical and chemical properties were made from an observatory carriage connected to a passenger train. Black carbon (BC) concentrations in fine particles (PM&lt;sub&gt;2.5&lt;/sub&gt;, aerodynamic diameter &amp;lt;2.5 μm) were measured with an aethalometer using a five-minute time resolution. Concentrations of inorganic ions and some organic compounds (Cl&lt;sup&gt;&amp;minus;&lt;/sup&gt;, NO&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt;&amp;minus;&lt;/sup&gt;, SO&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;2&amp;minus;&lt;/sup&gt;, Na&lt;sup&gt;+&lt;/sup&gt;, NH&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt;, K&lt;sup&gt;+&lt;/sup&gt;, Ca&lt;sup&gt;2+&lt;/sup&gt;, Mg&lt;sup&gt;2+&lt;/sup&gt;, oxalate and methane sulphonate) were measured continuously by using an on-line system with a 15-min time resolution. In addition, particle volume size distributions were determined for particles in the diameter range 3&amp;ndash;850 nm using a 10-min time resolution. The continuous measurements were completed with 24-h PM&lt;sub&gt;2.5&lt;/sub&gt; filter samples stored in a refrigerator and analyzed later in a chemical laboratory. The analyses included the mass concentrations of PM&lt;sub&gt;2.5&lt;/sub&gt;, ions, monosaccharide anhydrides (levoglucosan, galactosan and mannosan) and trace elements (Al, As, Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb, Sb, V and Zn). The mass concentrations of PM&lt;sub&gt;2.5&lt;/sub&gt; varied in the range of 4.3&amp;ndash;34.8 μg m&lt;sup&gt;&amp;minus;3&lt;/sup&gt; with an average of 21.6 μg m&lt;sup&gt;&amp;minus;3&lt;/sup&gt;. Fine particle mass consisted mainly of BC (average 27.6%), SO&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;2&amp;minus;&lt;/sup&gt; (13.0%), NH&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; (4.1%) and NO&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt;&amp;minus;&lt;/sup&gt; (1.4%). One of the major constituents was obviously organic carbon which was not determined. The contribution of BC was high compared with other studies made in Europe and Asia. High concentrations of ions, BC and particle volume were observed between Moscow and roughly 4000 km east of it, as well as close to Vladivostok, primarily due to local anthropogenic sources. In the natural background area between 4000 and 7200 km away from Moscow, observed concentrations were low, even though local particle sources, such as forest fires, occasionally increased concentrations. During the measured forest fire episodes, most of the aerosol mass appeared to consist of organic particulate matter. Concentrations of the biomass burning tracers levoglucosan, oxalate and potassium were elevated close to the forest fire areas observed by the MODIS satellite. The polluted air masses from Asia seem to have significant influences on the concentration levels of fine particles over south-eastern Russia

Chemical composition of atmospheric aerosols between Moscow and Vladivostok

International audienceThe TROICA-9 expedition (Trans-Siberian Observations Into the Chemistry of the Atmosphere) was carried out at the Trans-Siberian railway between Moscow and Vladivostok in October 2005. Measurements of aerosol physical and chemical properties were made from an observatory carriage connected to a passenger train. Black carbon (BC) concentrations in fine particles (PM2.5, aerodynamic diameter ?, NO3?, SO42?, Na+, NH4+, K+, Ca2+, Mg2+, oxalate and methane sulphonate) were measured continuously by using an on-line system with a 15-min time resolution. In addition, particle volume size distributions were determined for particles in the diameter range 3?850 nm using a 10-min. time resolution. The continuous measurements were completed with 24-h. PM2.5 filter samples which were stored in a refrigerator and later analyzed in chemical laboratory. The analyses included mass concentrations of PM2.5, ions, monosaccharide anhydrides (levoglucosan, galactosan and mannosan) and trace elements (Al, As, Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb, Sb, V and Zn). The mass concentrations of PM2.5 varied in the range of 4.3?34.8 ?g m?3 with an average of 21.6 ?g m?3. Fine particle mass consisted mainly of BC (average 27.6%), SO42? (13.0%), NH4+ (4.1%), and NO3? (1.4%). One of the major constituents was obviously also organic carbon which was not determined. The contribution of BC was high compared with other studies made in Europe and Asia. High concentrations of ions, BC and particle volume were observed between Moscow and roughly 4000 km east of it, as well as close to Vladivostok, primarily due to local anthropogenic sources. In the natural background area between 4000 and 7200 km distance from Moscow, observed concentrations were low, even though there were local particle sources, such as forest fires, that increased occasionally concentrations. The measurements indicated that during forest fire episodes, most of the aerosol mass consisted of organic particulate matter. Concentrations of biomass burning tracers levoglucosan, oxalate and potassium were elevated close to the forest fire areas observed by the MODIS satellite. The polluted air masses from Asia seem to have significant influences on the concentration levels of fine particles over south-eastern Russia

Continental impact on marine boundary layer coarse particles over the Atlantic Ocean between Europe and Antarctica

Aerosol samples were collected in the Atlantic marine boundary layer between the English Channel and Antarctica during November–December 1999. The composition of coarse (aerodynamic diameter 1–3 μm) individual aerosol particles was studied using the SEM/EDX method. The major particle types observed were fresh sea salt, sea-salt particles reacted partly or totally with sulphuric acid or nitric acid, Mg-sulphate, Ca-sulphate, mixed aluminosilicates and sea salt, aluminosilicates, Ca-rich particles and Fe-rich particles. The relative fractions of sea-salt particles with moderate or strong Cl depletion were high near the coasts of Europe (65–74%) and Northern Africa (44–87%), low far from the coast of Western Africa (10–20%) and very low in remote sea areas between Africa and Antarctica (1%). The Cl depletion was strongest when air masses arrived from the direction of anthropogenic pollution sources. The fractions of Mg-sulphate particles were high (18–25%) in 2 samples near Europe. The Mg-sulphate particles were probably formed as a result of fractional recrystallization of sea-salt particles in which Cl was substituted by sulphate. It remained unclear whether these particles were formed in the atmosphere or during and after sampling. The relative fractions of particles from continental sources were quite low (10–15%) near Europe, very high (25–78%) near the coast of Northwestern Africa and very low in the remote sea areas (0–2%). Most of the continental particles were aluminosilicates and some of them were internally mixed with sea salt. Near the coast of Northwestern Africa, the main source of aluminosilicates was Saharan dust, and near the Gulf of Guinea, emissions from biomass burning were also mixed with aluminosilicates and sea salt

Evaluation and modeling of the size fractionated aerosol number concentration measurements near a major road in Helsinki

Non peer reviewe

Evaluation and modeling of the size fractionated aerosol number concentration measurements near a major road in Helsinki

Non peer reviewe

Exhaust particle number and composition for diesel and gasoline passenger cars under transient driving conditions : Real-world emissions down to 1.5 nm

Recent recommendations given by WHO include systematic measurements of ambient particle number concentration and black carbon (BC) concentrations. In India and several other highly polluted areas, the air quality problems are severe and the need for air quality related information is urgent. This study focuses on particle number emissions and BC emissions of passenger cars that are technologically relevant from an Indian perspective. Particle number and BC were investigated under real-world conditions for driving cycles typical for Indian urban environments. Two mobile laboratories and advanced aerosol and trace gas instrumentation were utilized. Our study shows that passenger cars without exhaust particle filtration can emit in real-world conditions large number of particles, and especially at deceleration a significant fraction of particle number can be even in 1.5–10 nm particle sizes. The mass concentration of exhaust plume particles was dominated by BC that was emitted especially at acceleration conditions. However, exhaust particles contained also organic compounds, indicating the roles of engine oil and fuel in exhaust particle formation. In general, our study was motivated by serious Indian air quality problems, by the recognized lack of emission information related to Indian traffic, and by the recent WHO air quality guidance; our results emphasize the importance of monitoring particle number concentrations and BC also in Indian urban areas and especially in traffic environments where people can be significantly exposed to fresh exhaust emissions.Peer reviewe

Corrigendum to "Chemical characterization of springtime submicrometer aerosol in Po Valley, Italy" published in Atmos. Chem. Phys., 12, 8401–8421, 2012

No abstract available