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 reaction 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.

In spite of impressive advances in recent years, our present understanding of organic aerosol (OA) composition, physical and chemical properties, sources and transformation characteristics is still rather limited, and their environmental effects remain highly uncertain. This paper discusses and prioritizes issues related to organic aerosols and their effects on atmospheric processes and climate, providing a basis for future activities in the field. Four main topical areas are addressed: i) sources of OA; ii) formation transformation and removal of OA; iii) physical, chemical and mixing state of OA; iv) atmospheric modelling of OA. Key questions and research priorities regarding these four areas are synthesized in this paper, and outstanding issues for future research are presented for each topical area. In addition, an effort is made to formulate a basic set of consistent and universally applicable terms and definitions for coherent description of atmospheric OA across different scales and disciplines.

As demonstrated in a number of investigations, gaseous sulfuric acid plays a central role in atmospheric aerosol formation. Using chemical ionization mass spectrometer the gas-phase sulfuric acid and OH concentration were measured in Hyytiälä, SMEAR II station, Southern Finland during 24 March to 28 June 2007. Clear diurnal cycles were observed as well as differences between new particle formation event days and non-event days. Typically, the daily maximum concentrations of gas phase sulfuric acid varied from 3×10⁵ to 2×10⁶ molec cm⁻³ between non-event and event days. Noon-time OH concentrations varied from 3-6×10⁵ molec cm⁻³ and not a clear difference between event and non-events was detected. The measured time series were also used as a foundation to develop reasonable proxies for sulfuric acid concentration. The proxies utilized source and sink terms, and the simplest proxy is radiation times sulfur dioxide divided by condensation sink. Since it is still challenging to measure sulfuric acid in ambient concentrations, and due to its significant role in atmospheric particle formation, reasonable proxies are needed. We use all together three different proxies and one chemical box model and compared their results to the measured data. The proxies for the sulfuric acid concentration worked reasonably well, and will be used to describe sulfuric acid concentrations in SMEAR II station, when no measured sulfuric acid data is available. With caution the proxies could be applied to other environments as well.

The possible connections between the carbon balance of ecosystems and aerosol-cloud-climate interactions play a significant role in climate change studies. Carbon dioxide is a greenhouse gas, whereas the net effect of atmospheric aerosols is to cool the climate. Here, we investigated the connection between forest-atmosphere carbon exchange and aerosol dynamics in the continental boundary layer by means of multiannual data sets of particle formation and growth rates, of CO₂ fluxes, and of monoterpene concentrations in a Scots pine forest in southern Finland. We suggest a new, interesting link and a potentially important feedback among forest ecosystem functioning, aerosols, and climate: Considering that globally increasing temperatures and CO₂ fertilization are likely to lead to increased photosynthesis and forest growth, an increase in forest biomass would increase emissions of non-methane biogenic volatile organic compounds and thereby enhance organic aerosol production. This feedback mechanism couples the climate effect of CO₂ with that of aerosols in a novel way.

Because of the climate and air quality effects of organic aerosol, it is important to quantify the influence of anthropogenic emissions on the aerosol burden, both globally and regionally, and both in terms of mass and number. Methods exist with which the fractions of organic aerosol resulting directly from anthropogenic and biogenic processes can be estimated. However, anthropogenic emissions can also lead to an enhancement in secondary organic aerosol formation from naturally emitted precursors. We term this enhanced biogenic secondary organic aerosol (eBSOA). Here, we review the mechanisms through which such an effect may occur in the atmosphere and describe a work flow via which it may be quantified, using existing measurement techniques. An examination of published data reveals support for the existence of the enhancement effect.

Numerical models that combine weather forecasting and atmospheric chemistry are here referred to as chemical weather forecasting models. Eighteen operational chemical weather forecasting models on regional and continental scales in Europe are described and compared in this article. Topics discussed in this article include how weather forecasting and atmospheric chemistry models are integrated into chemical weather forecasting systems, how physical processes are incorporated into the models through parameterization schemes, how the model architecture affects the predicted variables, and how air chemistry and aerosol processes are formulated. In addition, we discuss sensitivity analysis and evaluation of the models, user operational requirements, such as model availability and documentation, and output availability and dissemination. In this manner, this article allows for the evaluation of the relative strengths and weaknesses of the various modelling systems and modelling approaches. Finally, this article highlights the most prominent gaps of knowledge for chemical weather forecasting models and suggests potential priorities for future research directions, for the following selected focus areas: emission inventories, the integration of numerical weather prediction and atmospheric chemical transport models, boundary conditions and nesting of models, data assimilation of the various chemical species, improved understanding and parameterization of physical processes, better evaluation of models against data and the construction of model ensembles.