An improved criterion for new particle formation in diverse atmospheric environments

A dimensionless theory for new particle formation (NPF) was developed, using an aerosol population balance model incorporating recent developments in nucleation rates and measured particle growth rates. Based on this theoretical analysis, it was shown that a dimensionless parameter <i>L</i><sub>Γ</sub>, characterizing the ratio of the particle scavenging loss rate to the particle growth rate, exclusively determined whether or not NPF would occur on a particular day. This parameter determines the probability that a nucleated particle will grow to a detectable size before being lost by coagulation with the pre-existing aerosol. Cluster-cluster coagulation was shown to contribute negligibly to this survival probability under conditions pertinent to the atmosphere. Data acquired during intensive measurement campaigns in Tecamac (MILAGRO), Atlanta (ANARChE), Boulder, and Hyytiälä (QUEST II, QUEST IV, and EUCAARI) were used to test the validity of <i>L</i><sub>Γ</sub> as an NPF criterion. Measurements included aerosol size distributions down to 3 nm and gas-phase sulfuric acid concentrations. The model was applied to seventy-seven NPF events and nineteen non-events (characterized by growth of pre-existing aerosol without NPF) measured in diverse environments with broad ranges in sulfuric acid concentrations, ultrafine number concentrations, aerosol surface areas, and particle growth rates (nearly two orders of magnitude). Across this diverse data set, a nominal value of <i>L</i><sub>Γ</sub>=0.7 was found to determine the boundary for the occurrence of NPF, with NPF occurring when <i>L</i><sub>Γ</sub><0.7 and being suppressed when <i>L</i><sub>Γ</sub>>0.7. Moreover, nearly 45% of measured <i>L</i><sub>Γ</sub> values associated with NPF fell in the relatively narrow range of 0.1<<i>L</i><sub>Γ</sub><0.3

Analyses of regulatory CD4(+)CD25(+)FOXP3(+) T cells and observations from peripheral T cell subpopulation markers during the development of type 1 diabetes in children

Our aim was to study whether the aberrant amount or function of regulatory T cells is related to the development of type 1 diabetes (T1D) in children. We also set out to investigate the balance of different T cell subtype markers during the T1D autoimmune process. Treg cells were quantified with flow cytometric assay, and the suppression capacity was analysed with a carboxyfluorescein succinimidyl ester (CFSE)-based T cell suppression assay in children in various phases of T1D disease process and in healthy autoantibody-negative control children. The mRNA expression of different T cell subpopulation markers was analysed with real-time qPCR method. The proportion and suppression capacity of regulatory T cells were similar in seroconverted children at an early stage of beta cell autoimmunity and also in children with T1D when compared to healthy and autoantibody-negative children. Significant differences were observed in the mRNA expression of different T cell subpopulation markers in prediabetic children with multiple (2) autoantibodies and in children with newly diagnosed T1D when compared to the control children. In conclusion, there were no quantitative or functional differences in regulatory T cells between the case and control groups in any phase of the autoimmune process. Decreased mRNA expression levels of T cell subtype markers were observed in children with multiple islet autoantibodies and in those with newly diagnosed T1D, probably reflecting an exhaustion of the immune system after the strong immune activation during the autoimmune process or a generally aberrant immune response related to the progression of the disease.Peer reviewe

Brightening of the global cloud field by nitric acid and the associated radiative forcing

Clouds cool Earth's climate by reflecting 20% of the incoming solar energy, while also trapping part of the outgoing radiation. The effect of human activities on clouds is poorly understood, but the present-day anthropogenic cooling via changes of cloud albedo and lifetime could be of the same order as warming from anthropogenic addition in CO<sub>2</sub>. Soluble trace gases can increase water condensation to particles, possibly leading to activation of smaller aerosols and more numerous cloud droplets. We have studied the effect of nitric acid on the aerosol indirect effect with the global aerosol-climate model ECHAM5.5-HAM2. Including the nitric acid effect in the model increases cloud droplet number concentrations globally by 7%. The nitric acid contribution to the present-day cloud albedo effect was found to be −0.32 W m<sup>−2</sup> and to the total indirect effect −0.46 W m<sup>−2</sup>. The contribution to the cloud albedo effect is shown to increase to −0.37 W m<sup>−2</sup> by the year 2100, if considering only the reductions in available cloud condensation nuclei. Overall, the effect of nitric acid can play a large part in aerosol cooling during the following decades with decreasing SO<sub>2</sub> emissions and increasing NO<sub>x</sub> and greenhouse gases

Analysis of nucleation events in the European boundary layer using the regional aerosol-climate model REMO-HAM with a solar radiation-driven OH-proxy

This work describes improvements in the regional aerosol–climate model REMO-HAM in order to simulate more realistically the process of atmospheric new particle formation (NPF). A new scheme was implemented to simulate OH radical concentrations using a proxy approach based on observations and also accounting for the effects of clouds upon OH concentrations. Second, the nucleation rate calculation was modified to directly simulate the formation rates of 3 nm particles, which removes some unnecessary steps in the formation rate calculations used earlier in the model. Using the updated model version, NPF over Europe was simulated for the periods 2003–2004 and 2008–2009. The statistics of the simulated particle formation events were subsequently compared to observations from 13 ground-based measurement sites. The new model shows improved agreement with the observed NPF rates compared to former versions and can simulate the event statistics realistically for most parts of Europe

New particle formation in air mass transported between two measurement sites in Northern Finland

This study covers four years of aerosol number size distribution data from Pallas and Värriö sites 250 km apart from each other in Northern Finland and compares new particle formation events between these sites. In air masses of eastern origin almost all events were observed to start earlier at the eastern station Värriö, whereas in air masses of western origin most of the events were observed to start earlier at the western station Pallas. This demonstrates that particle formation in a certain air mass type depends not only on the diurnal variation of the parameters causing the phenomenon (such as photochemistry) but also on some properties carried by the air mass itself. The correlation in growth rates between the two sites was relatively good, which suggests that the amount of condensable vapour causing the growth must have been at about the same level in both sites. The condensation sink was frequently much higher at the downwind station. It seems that secondary particle formation related to biogenic sources dominate in many cases over the particle sinks during the air mass transport between the sites. Two cases of transport from Pallas to Värriö were further analysed with an aerosol dynamics model. The model was able to reproduce the observed nucleation events 250 km down-wind at Värriö but revealed some differences between the two cases. The simulated nucleation rates were in both cases similar but the organic concentration profiles that best reproduced the observations were different in the two cases indicating that divergent formation reactions may dominate under different conditions. The simulations also suggested that organic compounds were the main contributor to new particle growth, which offers a tentative hypothesis to the distinct features of new particles at the two sites: Air masses arriving from the Atlantic Ocean typically spent approximately only ten hours over land before arriving at Pallas, and thus the time for the organic vapours to accumulate in the air and to interact with the particles is relatively short. This can lead to low nucleation mode growth rates and even to suppression of detectable particle formation event due to efficient scavenging of newly formed clusters, as was observed in the case studies

The contribution of boundary layer nucleation events to total particle concentrations on regional and global scales

International audienceThe contribution of boundary layer (BL) nucleation events to total particle concentrations on the global scale has been studied by including a new particle formation mechanism in a global aerosol microphysics model. The mechanism is based on an analysis of extensive observations of particle formation in the BL at a continental surface site. It assumes that molecular clusters form at a rate proportional to the gaseous sulfuric acid concentration to the power of 1. The formation rate of 3 nm diameter observable particles is controlled by the cluster formation rate and the existing particle surface area, which acts to scavenge condensable gases and clusters during growth. Modelled sulfuric acid vapour concentrations, particle formation rates, growth rates, coagulation loss rates, peak particle concentrations, and the daily timing of events in the global model agree well with observations made during a 22-day period of March 2003 at the SMEAR II station in Hyytiälä, Finland. The nucleation bursts produce total particle concentrations (>3 nm diameter) often exceeding 104 cm?3, which are sustained for a period of several hours around local midday. The predicted global distribution of particle formation events broadly agrees with what is expected from available observations. Over relatively clean remote continental locations formation events can sustain mean total particle concentrations up to a factor of 8 greater than those resulting from anthropogenic sources of primary organic and black carbon particles. However, in polluted continental regions anthropogenic primary particles dominate particle number and formation events lead to smaller enhancements of up to a factor of 2. Our results therefore suggest that particle concentrations in remote continental regions are dominated by nucleated particles while concentrations in polluted continental regions are dominated by primary particles. The effect of BL particle formation over tropical regions and the Amazon is negligible. These first global particle formation simulations reveal some interesting sensitivities. We show, for example, that significant reductions in primary particle emissions may lead to an increase in total particle concentration because of the coupling between particle surface area and the rate of new particle formation. This result suggests that changes in emissions may have a complicated effect on global and regional aerosol properties. Overall, our results show that new particle formation is a significant component of the aerosol particle number budget

Changes in background aerosol composition in Finland during polluted and clean periods studied by TEM/EDX individual particle analysis

Aerosol samples were collected at a rural background site in southern Finland in May 2004 during pollution episode ( PM1 similar to 16 mu g m(-3), backward air mass trajectories from south-east), intermediate period (PM1 similar to 5 mu g m(-3), backtrajectories from north-east) and clean period (PM1 similar to 2 mu g m(-3), backtrajectories from northwest/ north). The elemental composition, morphology and mixing state of individual aerosol particles in three size fractions were studied using transmission electron microscopy (TEM) coupled with energy dispersive X-ray (EDX) microanalyses. The TEM/EDX results were complemented with the size-segregated bulk chemical measurements of selected ions and organic and elemental carbon. Many of the particles in PM0.2-1 and PM1-3.3 size fractions were strongly internally mixed with S, C and/or N. The major particle types in PM0.2-1 samples were 1) soot and 2) ( ammonium) sulphates and their mixtures with variable amounts of C, K, soot and/or other inclusions. Number proportions of those two particle groups in PM0.2-1 samples were 0 - 12% and 83 - 97%, respectively. During the pollution episode, the proportion of Ca-rich particles was very high ( 26 - 48%) in the PM1- 3.3 and PM3.3-11 samples, while the PM0.2-1 and PM1- 3.3 samples contained elevated proportions of silicates ( 22 - 33%), metal oxides/hydroxides ( 1 - 9%) and tar balls ( 1 - 4%). These aerosols originated mainly from polluted areas of Eastern Europe, and some open biomass burning smoke was also brought by long-range transport. During the clean period, when air masses arrived from the Arctic Ocean, PM1- 3.3 samples contained mainly sea salt particles ( 67 - 89%) with a variable rate of Cl substitution ( mainly by NO3-). During the intermediate period, the PM1- 3.3 sample contained porous (sponge-like) Na-rich particles (35%) with abundant S, K and O. They might originate from the burning of wood pulp wastes of paper industry. The proportion of biological particles and C-rich fragments ( probably also biological origin) were highest in the PM3.3-11 samples ( 0 - 81% and 0 - 22%, respectively). The origin of different particle types and the effect of aging processes on particle composition and their hygroscopic and optical properties are discussed.Aerosol samples were collected at a rural background site in southern Finland in May 2004 during pollution episode ( PM1 similar to 16 mu g m(-3), backward air mass trajectories from south-east), intermediate period (PM1 similar to 5 mu g m(-3), backtrajectories from north-east) and clean period (PM1 similar to 2 mu g m(-3), backtrajectories from northwest/ north). The elemental composition, morphology and mixing state of individual aerosol particles in three size fractions were studied using transmission electron microscopy (TEM) coupled with energy dispersive X-ray (EDX) microanalyses. The TEM/EDX results were complemented with the size-segregated bulk chemical measurements of selected ions and organic and elemental carbon. Many of the particles in PM0.2-1 and PM1-3.3 size fractions were strongly internally mixed with S, C and/or N. The major particle types in PM0.2-1 samples were 1) soot and 2) ( ammonium) sulphates and their mixtures with variable amounts of C, K, soot and/or other inclusions. Number proportions of those two particle groups in PM0.2-1 samples were 0 - 12% and 83 - 97%, respectively. During the pollution episode, the proportion of Ca-rich particles was very high ( 26 - 48%) in the PM1- 3.3 and PM3.3-11 samples, while the PM0.2-1 and PM1- 3.3 samples contained elevated proportions of silicates ( 22 - 33%), metal oxides/hydroxides ( 1 - 9%) and tar balls ( 1 - 4%). These aerosols originated mainly from polluted areas of Eastern Europe, and some open biomass burning smoke was also brought by long-range transport. During the clean period, when air masses arrived from the Arctic Ocean, PM1- 3.3 samples contained mainly sea salt particles ( 67 - 89%) with a variable rate of Cl substitution ( mainly by NO3-). During the intermediate period, the PM1- 3.3 sample contained porous (sponge-like) Na-rich particles (35%) with abundant S, K and O. They might originate from the burning of wood pulp wastes of paper industry. The proportion of biological particles and C-rich fragments ( probably also biological origin) were highest in the PM3.3-11 samples ( 0 - 81% and 0 - 22%, respectively). The origin of different particle types and the effect of aging processes on particle composition and their hygroscopic and optical properties are discussed.Aerosol samples were collected at a rural background site in southern Finland in May 2004 during pollution episode ( PM1 similar to 16 mu g m(-3), backward air mass trajectories from south-east), intermediate period (PM1 similar to 5 mu g m(-3), backtrajectories from north-east) and clean period (PM1 similar to 2 mu g m(-3), backtrajectories from northwest/ north). The elemental composition, morphology and mixing state of individual aerosol particles in three size fractions were studied using transmission electron microscopy (TEM) coupled with energy dispersive X-ray (EDX) microanalyses. The TEM/EDX results were complemented with the size-segregated bulk chemical measurements of selected ions and organic and elemental carbon. Many of the particles in PM0.2-1 and PM1-3.3 size fractions were strongly internally mixed with S, C and/or N. The major particle types in PM0.2-1 samples were 1) soot and 2) ( ammonium) sulphates and their mixtures with variable amounts of C, K, soot and/or other inclusions. Number proportions of those two particle groups in PM0.2-1 samples were 0 - 12% and 83 - 97%, respectively. During the pollution episode, the proportion of Ca-rich particles was very high ( 26 - 48%) in the PM1- 3.3 and PM3.3-11 samples, while the PM0.2-1 and PM1- 3.3 samples contained elevated proportions of silicates ( 22 - 33%), metal oxides/hydroxides ( 1 - 9%) and tar balls ( 1 - 4%). These aerosols originated mainly from polluted areas of Eastern Europe, and some open biomass burning smoke was also brought by long-range transport. During the clean period, when air masses arrived from the Arctic Ocean, PM1- 3.3 samples contained mainly sea salt particles ( 67 - 89%) with a variable rate of Cl substitution ( mainly by NO3-). During the intermediate period, the PM1- 3.3 sample contained porous (sponge-like) Na-rich particles (35%) with abundant S, K and O. They might originate from the burning of wood pulp wastes of paper industry. The proportion of biological particles and C-rich fragments ( probably also biological origin) were highest in the PM3.3-11 samples ( 0 - 81% and 0 - 22%, respectively). The origin of different particle types and the effect of aging processes on particle composition and their hygroscopic and optical properties are discussed.Peer reviewe