ALBERT

Description: During the calendar years 1998-2002, 147 clear 8nm diameter particle formation events have been identified at the SMEAR I station in Värriö, northern Finland. The events have been classified in detail according to the particle formation rate, growth rate, event starting time, different trace gas concentrations and pre-existing particle concentrations as well as various meteorological conditions. The frequency of particle formation and growth events was highest during the spring months between March and May, suggesting that increasing biological activity might produce the precursor gases for particle formation. The apparent 8nm particle formation rates were around 0.1 /cm3s, and they were uncorrelated with growth rates that varied between 0.5 and 10nm/h. The air masses with clearly elevated sulphur dioxide concentrations (above 1.6ppb) came, as expected, from the direction of the Nikel and Monschegorsk smelters. Only 15 formation events can be explained by the pollution plume from these sources.

Description: As part of the OSOA (Origin and formation of Secondary Organic Aerosols) project, two intensive field campaigns were conducted in Melpitz, Germany and Hyytiälä, Finland. This paper gives an overview of the measurements made during the Hyytiälä campaign, which was held between 1 and 16 August 2001. Various instrumental techniques were used to achieve physical and chemical characterisation of aerosols and to investigate possible precursor gases. During the OSOA campaign in Hyytiälä, particle formation was observed on three consecutive days at the beginning of the campaign (1 to 3 August 2001) and on three days later on. The investigation of the meteorological situation divided the campaign into two parts. During the first three days of August, relatively cold and clean air masses from northwest passed over the station (condensation sink – CS:

Description: We carried out column model simulations to study particle fluxes and deposition and to evaluate different particle formation mechanisms at a boreal forest site in Finland. We show that kinetic nucleation of sulphuric acid cannot be responsible for new particle formation alone as the simulated vertical profile of particle number concentration does not correspond to observations. Instead organic induced nucleation leads to good agreement confirming the relevance of the aerosol formation mechanism including organic compounds emitted by the biosphere. The simulation of aerosol concentration within the atmospheric boundary layer during nucleation event days shows a highly dynamical picture, where particle formation is coupled with chemistry and turbulent transport. We have demonstrated the suitability of our turbulent mixing scheme in reproducing the most important characteristics of particle dynamics within the boundary layer. Deposition and particle flux simulations show that deposition affects noticeably only the smallest particles in the lowest part of the atmospheric boundary layer.

Description: Night-time ozone deposition for a Scots pine forest in Southern Finland was studied at the SMEAR II measurement station by evaluating the turbulent eddy covariance (EC), storage change and vertical advection fluxes. Similarly to night-time carbon dioxide flux, the eddy-covariance flux of ozone was decreasing with turbulence intensity (friction velocity), and storage change of the compound did not compensate the reduction (well-known night-time measurement problem). Accounting for vertical advection resulted in invariance of ozone deposition rate on turbulence intensity. This was also demonstrated for carbon dioxide, verified by independent measurements of NEE by chamber systems. The result highlights the importance of advection when considering the exchange measurements of any scalar. Analysis of aerodynamic and laminar boundary layer resistances by the model approach indicated that the surface resistance and/or chemical sink strength was limiting ozone deposition. The possible aerial ozone sink by known fast chemical reactions with sesquiterpenes and NO explain only a minor fraction of ozone sink. Thus the deposition is controlled either by stomatal uptake or surface reactions or both of them, the mechanisms not affected by turbulence intensity. Therefore invariance of deposition flux on turbulence intensity is expected also from resistance and chemical sink analysis.

Description: 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.

Description: We have carried out an inter-comparison between EddyUH and EddyPro®, two public software packages for post-field processing of eddy covariance data. Datasets including carbon dioxide, methane and water vapour fluxes measured over two months at a wetland in Southern Finland and carbon dioxide and water vapour fluxes measured over three months at an urban site in Helsinki, were processed and analysed. The purpose was to estimate the flux uncertainty due to the use of different software packages and to evaluate the most critical processing steps, determining the largest deviations in the calculated fluxes. Turbulent fluxes calculated with a reference combination of processing steps were in good agreement, the systematic difference between the two software packages being up to 2% and 6.7% for half-hour and cumulative sum values, respectively. The raw data preparation and processing steps were consistent between the software packages, and most of the deviations in the estimated fluxes were due to the flux corrections. Among the different calculation procedures analysed, the spectral correction had biggest impact for closed-path latent heat fluxes, reaching nocturnal median value of 15% at the wetland site. We found up to 43% median value of deviation (with respect to the run with all corrections included) if closed path carbon dioxide flux is calculated without the dilution correction, while the methane fluxes were up to 10% lower without both dilution and spectroscopic corrections. The density (and spectroscopic) correction was the most critical step for open-path systems. However, we found also large spectral correction factors for the open-path methane fluxes, due to the sensor separation effect.

Description: Long-term eddy covariance particle number flux measurements for the diameter range 6 nm to 5 μm were performed at the SMEAR III station over an urban area in Helsinki, Finland. The heterogeneity of the urban measurement location allowed us to study the effect of different land-use classes in different wind directions on the measured fluxes. The particle number fluxes were highest in the direction of a local road on weekdays, with a daytime median flux of 0.8×109 m−2 s−1. The particle fluxes showed a clear dependence on traffic rates and on the mixing conditions of the boundary layer. The measurement footprint was estimated by the use of both numerical and analytical models. Using the crosswind integrated form of the footprint function, we estimated the emission factor for the mixed vehicle fleet, yielding a median particle number emission factor per vehicle of 3.0×1014 # km−1. Particle fluxes from the vegetated area were the lowest with daytime median fluxes below 0.2×109 m−2 s−1. During weekends and nights, the particle fluxes were low from all land use sectors being in the order of 0.02–0.1×109 m−2 s−1. On an annual scale the highest fluxes were measured in winter, when emissions from stationary combustion sources are also highest. Particle number fluxes were compared with the simultaneously measured CO2 fluxes and similarity in their sources was distinguishable. For CO2, the median emission factor of vehicles was estimated to be 370 g km−1.

Description: This study scrutinizes a decade-long series of ozone deposition measurements in a boreal forest in search for the signature and relevance of the different deposition processes. The canopy-level ozone flux measurements were analysed for deposition characteristics and partitioning into stomatal and non-stomatal fractions, with the main focus on growing season day-time data. Ten years of measurements enabled the analysis of ozone deposition variation at different time-scales, including daily to inter-annual variation as well as the dependence on environmental variables and concentration of biogenic volatile organic compounds (BVOC-s). Stomatal deposition was estimated by using multi-layer canopy dispersion and optimal stomatal control modelling from simultaneous carbon dioxide and water vapour flux measurements, non-stomatal was inferred as residual. Also, utilising the big-leaf assumption stomatal conductance was inferred from water vapour fluxes for dry canopy conditions. The total ozone deposition was highest during the peak growing season (4 mm s−1) and lowest during winter dormancy (1 mm s−1). During the course of the growing season the fraction of the non-stomatal deposition of ozone was determined to vary from 26 to 44% during day time, increasing from the start of the season until the end of the growing season. By using multi-variate analysis it was determined that day-time total ozone deposition was mainly driven by photosynthetic capacity of the canopy, vapour pressure deficit (VPD), photosynthetically active radiation and monoterpene concentration. The multi-variate linear model explained the high portion of ozone deposition variance on daily average level (R2 = 0.79). The explanatory power of the multi-variate model for ozone non-stomatal deposition was much lower (R2 = 0.38). The set of common environmental variables and terpene concentrations used in multivariate analysis were able to predict the observed average seasonal variation in total and non-stomatal deposition but failed to explain the inter-annual differences, suggesting that some still unknown mechanisms might be involved in determining the inter-annual variability. Model calculation was performed to evaluate the potential sink strength of the chemical reactions of ozone with sesquiterpenes in the canopy air space, which revealed that sesquiterpenes in typical amounts at the site were unlikely to cause significant ozone loss in canopy air space. The results clearly showed the importance of several non-stomatal removal mechanisms. Unknown chemical compounds or processes correlating with monoterpene concentrations, including potentially reactions at the surfaces, contribute to non-stomatal sink term.

Description: In the analyses of VOC fluxes measured above plant canopies, one usually assumes the flux above canopy to equal the exchange at the surface. Thus one assumes the chemical degradation to be much slower than the turbulent transport. We used a stochastic Lagrangian transport model in which the chemical degradation was described as first order decay in order to study the effect of the chemical degradation on above canopy fluxes of chemically reactive species. With the model we explored the sensitivity of the ratio of the above canopy flux to the surface emission on several parameters such as chemical lifetime of the compound, friction velocity, stability, and canopy density. Our results show that friction velocity and chemical lifetime affected the loss during transport the most. The canopy density had a significant effect if the chemically reactive compound was emitted from the forest floor. We used the results of the simulations together with oxidant data measured during HUMPPA-COPEC-2010 campaign at a Scots pine site to estimate the effect of the chemistry on fluxes of three typical biogenic VOCs, isoprene, α-pinene, and β-caryophyllene. Of these, the chemical degradation had a major effect on the fluxes of the most reactive species β-caryophyllene, while the fluxes of α-pinene were affected during nighttime. For these two compounds representing the mono- and sesquiterpenes groups, the effect of chemical degradation had also a significant diurnal cycle with the highest chemical loss at night. The different day and night time loss terms need to be accounted for, when measured fluxes of reactive compounds are used to reveal relations between primary emission and environmental parameters.

Description: This study scrutinizes a decade-long series of ozone deposition measurements in a boreal forest in search for the signature and relevance of the different deposition processes. Canopy-level ozone flux measurements were analysed for deposition characteristics and partitioning into stomatal and non-stomatal fractions, focusing on growing season day-time data. Ten years of measurements enabled the analysis of ozone deposition variation at different time- scales, including daily to inter-annual variation as well as the dependence on environmental variables and concentration of biogenic volatile organic compounds (BVOC-s). Stomatal deposition was estimated by using multi-layer canopy dispersion and optimal stomatal control modelling from simultaneous carbon dioxide and water vapour flux measurements, non-stomatal was inferred as residual. Also, utilising big-leaf assumption stomatal conductance was inferred from water vapour fluxes for dry canopy conditions. The total ozone deposition was highest during the peak growing season (4 mm s−1) and lowest during winter dormancy (1 mm s−1). During the course of the growing season the fraction of the non-stomatal deposition of ozone was determined to vary from 26 to 44% during day time, increasing from the start of the season until the end of the growing season. By using multi-variate analysis it was determined that day-time total ozone deposition was mainly driven by photosynthetic capacity of the canopy, vapour pressure deficit (VPD), photosynthetically active radiation and monoterpene concentration. The multi-variate linear model explained high portion of ozone deposition variance on daily average level (R2 = 0.79). The explanatory power of the multi-variate model for ozone non-stomatal deposition was much lower (R2 = 0.38). Model calculation was performed to evaluate the potential sink strength of the chemical reactions of ozone with sesquiterpenes in the canopy air space, which revealed that sesquiterpenes in typical amounts at the site were unlikely to cause significant ozone loss in canopy air space. This was also confirmed by the statistical analysis that did not link measured sesquiterpene concentration with ozone deposition. It was concluded that chemical reactions with monoterpenes, or other removal mechanisms such as surface reactions, play a role as ozone non-stomatal sink inside canopy.