Abstract.We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiälä (Finland). During the campaign numerous aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth (to a diameter of 3 nm) of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two when the time delay between the sulphuric acid and particle number concentration is taken into account. From the time delay the growth rates of freshly nucleated particles from 1 nm to 3 nm were determined. The mean growth rate was 1.2 nm/h and it was clearly correlated with the gaseous sulphuric acid concentration. We tested two nucleation mechanisms -recently proposed cluster activation and kinetic type nucleation -as possible candidates to explain the observed dependences, and determined experimental nucleation coefficients. We found that some events are dominated by the activation mechanism and some by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are the same order of magnitude as chemical re-action coefficients in the gas phase and they correlate with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation.

Abstract. 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 ([H 2 SO 4 ]), and particle concentrations (N 3−6 ) or formation rates at 1 nm and 3 nm (J 1 and J 3 ); 2) the time delays between [H 2 SO 4 ] and N 3−6 or J 3 , and the growth rates for 1-3 nm particles; 3) the empirical nucleation coefficients A and K in relations J 1 =A[H 2 SO 4 ] and J 1 =K[H 2 SO 4 ] 2 , respectively; 4) theoretical predictions for J 1 and J 3 for the days when no significant particle formation is observed, based on the observed sulphuric acid concentrations and condensation sinks. In both environments, N 3−6 or J 3 and [H 2 SO 4 ] 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 J 3 and [H 2 SO 4 ] were consistently lower than the corresponding Correspondence to: I. Riipinen (ilona.riipinen@helsinki.fi) delays between N 3−6 and [H 2 SO 4 ]. The exponents in the J 3 ∝[H 2 SO 4 ] n J 3 -connection were consistently higher than or equal to the exponents in the relation N 3−6 ∝[H 2 SO 4 ] n N36 . In the J 1 values, no significant differences were found between the observed rates on particle formation event days and the predictions on non-event days. The J 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.

Abstract. A large number of oxygenated organic chemicals (peroxyacyl nitrates, alkyl nitrates, acetone, formaldehyde, methanol, methylhydroperoxide, acetic acid and formic acid) were measured during the 1997 Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) airborne field campaign over the Atlantic. In this paper, we present a first picture of the distribution of these oxygenated organic chemicals (Ox-organic) in the troposphere and the lower stratosphere, and assess their source and sink relationships. In both the troposphere and the lower stratosphere, the total atmospheric abundance of these oxygenated species (ZOx-organic) nearly equals that of total nonmethane hydrocarbons (ZNMHC), which have been traditionally measured.

[1] In this paper we present simulations with a Lagrangian particle dispersion model to study the intercontinental transport of pollution from North America during an aircraft measurement campaign over Europe. The model was used for both the flight planning and a detailed source analysis after the campaign, which is described here with examples from two episodes. Forward calculations of emission tracers from North America, Europe, and Asia were made in order to understand the transport processes. Both episodes were preceded by stagnant conditions over North America, leading to the accumulation of pollutants in the North American boundary layer. Both anthropogenic sources and, to a lesser extent, forest fire emissions contributed to this pollution, which was then exported by warm conveyor belts to the middle and upper troposphere, where it was transported rapidly to Europe. Concentrations of many trace gases (CO, NO y , CO 2 , acetone, and several volatile organic compounds; O 3 in one case) and of ambient atmospheric ions measured aboard the research aircraft were clearly enhanced in the pollution plumes compared to the conditions outside the plumes. Backward simulations with the particle model were introduced as an indispensable tool for a more detailed analysis of the plume's source region. They make trajectory analyses (which, to date, were mainly used to interpret aircraft measurement data) obsolete. Using an emission inventory, we could decompose the tracer mixing ratios at the receptors (i.e., along the flight tracks) into contributions from every grid cell of the inventory. For both plumes we found that emission sources contributing to the tracer concentrations over Europe were distributed over large areas in North America. In one case, sources in California, Texas, and Florida contributed almost equally, and smaller contributions were also made by other sources located between the Yucatan Peninsula and Canada. In the other case, sources in eastern North America, including moderate contributions from forest fires, were most important. The plume's maximum was mainly caused by anthropogenic emissions from the New York area. To our knowledge, this is the first case reported where a pollution plume from a megacity was reliably detected over another continent.

The family Rhizobiaceae contains plant-associated bacteria with critical roles in ecology and agriculture. Within this family, many Rhizobium and Sinorhizobium strains are nitrogen-fixing plant mutualists, while many strains designated as Agrobacterium are plant pathogens. These contrasting lifestyles are primarily dependent on the transmissible plasmids each strain harbors. Members of the Rhizobiaceae also have diverse genome architectures that include single chromosomes, multiple chromosomes, and plasmids of various sizes. Agrobacterium strains have been divided into three biovars, based on physiological and biochemical properties. The genome of a biovar I strain, A. tumefaciens C58, has been previously sequenced. In this study, the genomes of the biovar II strain A. radiobacter K84, a commercially available biological control strain that inhibits certain pathogenic agrobacteria, and the biovar III strain A. vitis S4, a narrow-host-range strain that infects grapes and invokes a hypersensitive response on nonhost plants, were fully sequenced and annotated. Comparison with other sequenced members of the Alphaproteobacteria provides new data on the evolution of multipartite bacterial genomes. Primary chromosomes show extensive conservation of both gene content and order. In contrast, secondary chromosomes share smaller percentages of genes, and conserved gene order is restricted to short blocks. We propose that secondary chromosomes originated from an ancestral plasmid to which genes have been transferred from a progenitor primary chromosome. Similar patterns are observed in select Beta-and Gammaproteobacteria species. Together, these results define the evolution of chromosome architecture and gene content among the Rhizobiaceae and support a generalized mechanism for second-chromosome formation among bacteria.The family Rhizobiaceae (order Rhizobiales) of the Alphaproteobacteria includes the plant pathogens of the genus Agrobacterium and the nitrogen-fixing plant mutualists of the genera Rhizobium and Sinorhizobium. Members house single and multiple chromosome arrangements, linear replicons, and plasmids of various sizes. Genes of pathogenicity, mutualism, and other symbiotic properties are primarily encoded on large transmissible plasmids. Given the promiscuous nature of these elements, different genomic lineages within the Rhizobiaceae exhibit a variety of symbiotic phenotypes that range from pathogenesis to nitrogen-fixing mutualism.Agrobacterium taxonomy and phylogeny display a marked disparity. Empirically, organisms of the genus Agrobacterium are grouped into five species based on the disease phenotype associated with the resident disease-inducing plasmid: A. tumefaciens causes crown gall on dicotyledonous plants, including stone fruit and nut trees; A. rubi causes crown gall on raspberries; A. vitis causes gall formation that is limited to grapes; A. rhizogenes causes hairy root disease; and A. radiobacter is avirulent. An alternative classification scheme

This manuscript gives an up-to-date and comprehensive overview of the effects of energetic particle precipitation (EPP) onto the whole atmosphere, from the lower thermosphere/mesosphere through the stratosphere and troposphere, to the surface. The paper summarizes the different sources and energies of particles, principally galactic cosmic rays (GCRs), solar energetic particles (SEPs) and energetic electron precipitation (EEP). All the proposed mechanisms by which EPP can affect the atmosphere are discussed, including chemical changes in the upper atmosphere and lower thermosphere, chemistry-dynamics feedbacks, the global electric circuit and cloud formation. The role of energetic particles in Earth's atmosphere is a multi-disciplinary problem that requires expertise from a range of scientific backgrounds. To assist with this synergy, summary tables are provided, which are intended to evaluate the level of current knowledge of the effects of energetic particles on processes in the entire atmosphere.

Abstract. Gaseous sulphuric acid is a key precursor for new particle formation in the atmosphere. Previous experimental studies have confirmed a strong correlation between the number concentrations of freshly formed particles and the ambient concentrations of sulphuric acid. This study evaluates a body of experimental gas phase sulphuric acid concentrations, as measured by Chemical Ionization Mass Spectrometry (CIMS) during six intensive measurement campaigns and one long-term observational period. The campaign datasets were measured in Hyytiälä,

Abstract. Aerosol physical and chemical properties and trace gas concentrations were measured during the QUEST field campaign in March-April 2003, in Hyytiälä, Finland. Our aim was to understand the role of oxidation products of VOC's such as mono-and sesquiterpenes in atmospheric nucleation events. Particle chemical compositions were measured using the Aerodyne Aerosol Mass Spectrometer, and chemical compositions of aerosol samples collected with low-pressure impactors and a high volume sampler were analysed using a number of techniques. The results indicate that during and after new particle formation, all parti-cles larger than 50 nm in diameter contained similar organic substances that are likely to be mono-and sesquiterpene oxidation products. The oxidation products identified in the high volume samples were shown to be mostly aldehydes. In order to study the composition of particles in the 10-50 nm range, we made use of Tandem Differential Mobility Analyzer results. We found that during nucleation events, both 10 and 50 nm particle growth factors due to uptake of ethanol vapour correlate strongly with gas-phase monoterpene oxidation product (MTOP) concentrations, indicating that the organic constituents of particles smaller than 50 nm in diameter are at least partly similar to those of larger particles. We furthermore showed that particle growth rates during the nucleation events are correlated with the gas-phase MTOP Published by Copernicus Publications on behalf of the European Geosciences Union. 2658A. Laaksonen et al.: VOC oxidation products and new particle formation concentrations. This indicates that VOC oxidation products may have a key role in determining the spatial and temporal features of the nucleation events. This conclusion was supported by our aircraft measurements of new 3-10 nm particle concentrations, which showed that the nucleation event on 28 March 2003, started at the ground layer, i.e. near the VOC source, and evolved together with the mixed layer. Furthermore, no new particle formation was detected upwind away from the forest, above the frozen Gulf of Bothnia.