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A few studies on ozone deposition over lake water are available and so far only one using the eddy covariance technique (Wesely et al., 1981, https://doi.org/10.1007/BF00122295). A 23‐day field campaign was held in August‐September 2012 at the Lake Kuivajärvi in Hyytiälä, Finland. The results showed a mean flux of −30 ± 1 ng m−2 s−1 and deposition velocity of 0.86 ± 0.05 mm s−1. Deposition velocity showed a weak diurnal cycle over the lake with elevated values during the nighttime. The daytime and nighttime portions of the data set differed statistically. Analysis showed that waterside convective mixing enhanced deposition and such conditions pre‐dominantly occurred during nighttime. We compared the measured deposition velocities with the dry deposition model of air‐sea exchange, adjusted for the chemical sinks relevant for the lake. We suggest that the buoyant mixing and unaccounted chemistry can be responsible for the difference between the model results and observations. Plain Language Summary: Ozone deposition was studied over lake in Southern Finland. Deposition velocity showed elevated values during the nighttime. Higher ozone deposition at night was related to enhanced convective mixing in uppermost water layers. Key Points: Ozone deposition over the lake is enhanced by waterside buoyancy velocityWind speed and friction velocity had minor or no impact on ozone deposition, instead waterside convective mixing enhanced depositionIn late summer, over diurnal course higher deposition velocities occurred at night [ABSTRACT FROM AUTHOR]

One dimensional atmospheric boundary layer (ABL) model coupled with detailed atmospheric chemistry and aerosol dynamical model, the model SOSAA, was used to predict the ABL and detailed aerosol population (characterized by the number size distribution) time evolution. The model was applied over a period of ten days in May 2013 for a pine forest site in southern Finland. The period was characterized by frequent new particle formation events and simultaneous intensive aerosol transformation. Throughout this study we refer to nucleation, condensational growth and coagulation as aerosol dynamical processes, i.e. the processes that govern the particle size distribution evolution. The aim of the study was to analyze and quantify the role of aerosol and ABL dynamics in vertical transport of aerosols. It was of particular interest to what extent the fluxes above canopy deviate due to above mentioned processes from the particle dry deposition on the canopy foliage. The model simulations revealed that the particle concentration change due to aerosol dynamics can frequently exceed the effect of particle deposition even an order of magnitude or more. The impact is however strongly dependent on particle size and time. In spite of the fact that the time scale of turbulent transfer inside canopy is much smaller than the time scales of aerosol dynamics and dry deposition, letting to assume well mixed properties of air, the fluxes at the canopy top frequently deviate from deposition inside forest. This is due to transformation of aerosol concentration throughout the ABL and resulting complicated pattern of vertical transport. Therefore we argue that the comparison of time scales of aerosol dynamics and deposition defined for the processes below the flux measurement level do not unambiguously describe the importance of aerosol dynamics for vertical transport within canopy. We conclude that under dynamical conditions the micrometeorological particle flux measurements such as performed by the eddy covariance technique do not generally represent the dry deposition. The deviation can be systematic for certain size ranges so that the conclusion applies also to time averaged particle fluxes. [ABSTRACT FROM AUTHOR]

Four gas analysers capable of measuring nitrous oxide (N2 concentration at a response time necessary for eddy covariance flux measurements were operated from spring until winter 2011 over a field cultivated with reed canary grass (RCG, Phalaris arundinacea, L.), a perennial bioenergy crop in eastern Finland. The instruments were TGA100A (Campbell Scientific Inc.), CW-TILDAS-CS (Aerodyne Research Inc.), N2O / CO-23d (Los Gatos Research Inc.) and QC-TILDAS-76-CS (Aerodyne Research Inc.). The period with high emissions, lasting for about 2 weeks after fertilization in late May, was characterized by an up to 2 orders of magnitude higher emission, whereas during the rest of the campaign the N2O fluxes were small, from 0.01 to 1 nmol m-2 s-1 instruments, CW-TILDAS-CS and N2O / CO-23d, determined the N2O exchange with minor systematic difference throughout the campaign, when operated simultaneously. TGA100A produced the cumulatively highest N2O estimates (with 29% higher values during the period when all instruments were operational). QC-TILDAS-76-CS obtained 36% lower fluxes than CW-TILDAS-CS during the first period, including the emission episode, whereas the correspondence with other instruments during the rest of the campaign was good. The reasons for systematic differences were not identified, suggesting further need for detailed evaluation of instrument performance under field conditions with emphasis on stability, calibration and any other factors that can systematically affect the accuracy of flux measurements. The instrument CW-TILDAS-CS was characterized by the lowest noise level (with a standard deviation of around 0.12 ppb at 10 Hz sampling rate) as compared to N2O / CO-23d and QC-TILDAS-76-CS (around 0.50 ppb) and TGA100A (around 2 ppb). We identified that for all instruments except CW-TILDAS-CS the random error due to instrumental noise was an important source of uncertainty at the 30 min averaging level and the total stochastic error was frequently of the same magnitude as the fluxes when N2O exchange was small at the measurement site. Both instruments based on continuous-wave quantum cascade laser, CW-TILDAS-CS and N2O / CO-23d, were able to determine the same sample of low N2O fluxes with a high mutual coefficient of determination at the 30 min averaging level and with minor systematic difference over the observation period of several months. This enables us to conclude that the new-generation instrumentation is capable of measuring small N2O exchange with high precision and accuracy at sites with low fluxes. [ABSTRACT FROM AUTHOR]

Four gas analysers capable of measuring nitrous oxide (N2O) concentration at a response time necessary for eddy covariance flux measurements were operated from spring till winter 2011 over a field cultivated with reed canary grass (RCG, Phalaris arundinaceae, L.), a perennial bioenergy crop in Eastern Finland. The instruments were TGA100A (Campbell Scientific Inc.), CW-TILDAS-CS (Aerodyne Research Inc.), N2O/CO-23d (Los Gatos Research Inc.) and QC-TILDAS-76-CS (Aerodyne Research Inc.). The period with high emission, lasting for about two weeks after fertilization in late May, was characterised by an up to two orders of magnitude higher emission, whereas during the rest of the campaign the N2O fluxes were small, from 0.1 to 1 nmol m-2 s-1. Two instruments, CW-TILDAS-CS and N2O/CO-23d, determined the N2O exchange with minor systematic difference throughout the campaign, when operated simultaneously. TGA100A produced cumulatively highest N2O estimates (with 29% higher value during the period when all instruments were operational). QC-TILDAS-76-CS obtained 36% lower fluxes than CW-TILDAS-CS during the first period, including the emission episode, whereas the correspondence with other instruments during the rest of the campaign was good. The reason for these episodic higher and lower estimates by the two instruments is not currently known, suggesting further need for detailed evaluation of instrument performance under field conditions with emphasis on stability, calibration and, in particular, simultaneous accurate determination of water vapour concentration due to its large impact on small N2O fluxes through spectroscopic and dilution corrections. The instrument CW-TILDAS-CS was characterised by the lowest noise level (std around 0.12 ppb at 10Hz sampling rate), as compared to N2O/CO-23d and QC-TILDAS-76-CS (around 0.50 ppb) and TGA100A (around 2 ppb). Both instruments based on Continuous-Wave Quantum Cascade Lasers, CW-TILDAS-CS and N2O/CO-23d, were able to determine the same sample of low N2O fluxes with high mutual coefficient of determination at 30min averaging level and with minor systematic difference over the observation period of several months. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

In the analyses of VOC fluxes measured above plant canopies, one usually assumes the flux above canopy to equal the emission 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 HUMPPACOPEC- 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. [ABSTRACT FROM AUTHOR]

Eddy covariance (EC) flux measurements of nitrous oxide (N2O) obtained by using a 3-D sonic anemometer and a tunable diode laser gas analyzer for N2O were investigated. Two datasets (Sorø, Denmark and Kalevansuo, Finland) from different measurement campaigns including subcanopy flux measurements of energy and carbon dioxide are discussed with a focus on selected quality control aspects and flux error analysis. Although fast response trace gas analyzers based on spectroscopic techniques are increasingly used in ecosystem research, their suitability for reliable estimates of EC fluxes is still limited, and some assumptions have to be made for filtering and processing data. The N2O concentration signal was frequently dominated by offset drifts (fringe effect), which can give an artificial extra contribution to the fluxes when the resulting concentration fluctuations are correlated with the fluctuations of the vertical wind velocity. Based on Allan variance analysis of the N2O signal, we found that a recursive running mean filter with a time constant equal to 50 s was suitable to damp the influence of the periodic drift. Although the net N2O fluxes over the whole campaign periods were quite small at both sites (∼ 5 μgNm-2 h-1 for Kalevansuo and ∼ 10 μgNm-2 h-1 for Sorø), the calculated sub-canopy EC fluxes were in good agreement with those estimated by automatic soil chambers. However, EC N2O flux measurements show larger random uncertainty than the sensible heat fluxes, and classification according to statistical significance of single flux values indicates that downward N2O fluxes have larger random error. [ABSTRACT FROM AUTHOR]

Long-term eddy covariance particle number flux measurements for the diameter range 6 nm to 5μm 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. [ABSTRACT FROM AUTHOR]

Eddy covariance (EC) flux measurements of nitrous oxide obtained by using a 3-D sonic anemometer and a tunable diode laser gas analyzer for N2O were investigated. Two datasets (Sorø, Denmark and Kalevansuo, Finland) from different measurement campaigns including sub-canopy flux measurements of energy and carbon dioxide are discussed with a focus on selected quality control aspects and flux error analysis. Although fast response trace gas analyzers based on spectroscopic techniques are increasingly used in ecosystem research, their suitability for reliable estimates of eddy covariance fluxes is still limited, and some assumptions have to be made for filtering and processing data. The N2O concentration signal was frequently dominated by offset drifts (fringe effect), which can give an artificial extra contribution to the fluxes when the resulting concentration fluctuations are correlated with the fluctuations of the vertical wind velocity. Based on Allan variance analysis of the N2O signal, we found that a recursive running mean filter with a time constant equal to 50s was suitable to damp the influence of the periodic drift. Although the net N2O fluxes over the whole campaign periods were quite small at both sites (∼5 μgNm-2 h-1 for Kalevansuo and ∼10 μgNm-2 h-1 for Sorø), the calculated sub-canopy EC fluxes were in good agreement with those estimated by automatic soil chambers. However EC N2O flux measurements show larger random uncertainty than the sensible heat fluxes, and classification according to statistical significance of single flux values indicates that downward N2O fluxes have larger random error. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Of the 60% of particle number fluxes over two forests that exceed the associated uncertainty bounds, approximately one-third are upward. These ‘apparent emission’ fluxes are not solely observed during periods when other micro-meteorological fluxes are ill-defined, which implies they derive from a/multiple physical cause/s. Upward fluxes are slightly more frequent at night over the Danish beech forest but do not depend on wind direction or speed. Data from the pine forest in Finland indicate no diurnal cycle in the frequency with which upward fluxes are observed, although as in data from the beech forest the magnitude of upward fluxes is higher during the day. At the pine forest local emissions may account for some of the upward fluxes but other mechanisms appear also to play a role. Entrainment of particle depleted air from above the boundary layer, analysed via use of quadrant analysis and scalar correlations, appears to be important in the occurrence of upward fluxes at both sites. The rate of upward fluxes scales with prevailing geometric mean diameter (GMD) and consistent with the hypothesis of entrainment of relatively particle-depleted air upward fluxes appear to be associated with particle ensembles characterized by larger prevailing GMD. [ABSTRACT FROM AUTHOR]

Thinning is a routine forest management operation that changes tree spacing, number, and size distribution and affects the material flows between vegetation and the atmosphere. Here, using direct micrometeorological ecosystem-scale measurements, we show that in a boreal pine forest, thinning decreases the deposition velocities of fine particles as expected but does not reduce the carbon sink, water vapor flux, or ozone deposition. The thinning decreased the all-sided leaf area index from 8 to 6, and we suggest that the redistribution of sources and sinks within the ecosystem compensated for this reduction in foliage area. In the case of water vapor and 03, changes in light penetration and among-free competition seem to increase individual transpiration rates and lead to larger stomatal apertures, thus enhancing also O3 deposition. In the case of CO2, increased ground vegetation assimilation and decreased autotrophic respiration seem to cancel out opposite changes in canopy assimilation and heterotrophic respiration. Current soil-vegetation-atmosphere transfer models should be able to reproduce these observations. [ABSTRACT FROM AUTHOR]

Spring time soil nitrous oxide (N2O) fluxes were measured in an old beech (Fagus sylvatica L.) forest with eddy covariance (EC) and chamber techniques. The aim was to compare the two techniques and to test whether EC can be used in the trunk-space of the forest to measure N2O. Mean N2O fluxes over the five week measurement period were 5, 10 and 16 µg N m-2 h-1 from EC, automatic chamber and manual chambers, respectively. When data from one hot spot chamber was excluded the mean N2O flux of 8 µg N m-2h-1 from the soil chambers nearly equaled to the mean flux of 7 µg N m-2 h-1 measured with EC from the direction were soil chambers located. Spatial variability in the N2O emissions was high in soil chamber measurements, while the EC integrated over this spatial variability and suggested that N2O emissions were uniform within the footprint area. The highest emissions measured with the EC occurred during the first week of May when the trees were leafing and when soil moisture content was at its highest. To our knowledge, this is the first study to demonstrate that the EC technique can be used to measure N2O fluxes in the trunk-space of a forest. If chamber techniques are used to estimate ecosystem level N2O emissions from forest soils, placing of the chambers should be considered carefully to cover the heterogeneity in the soil N2O emissions. [ABSTRACT FROM AUTHOR]

Summary This paper presents CO2 flux data from 18 forest ecosystems, studied in the European Union funded EUROFLUX project. Overall, mean annual gross primary productivity (GPP, the total amount of carbon (C) fixed during photosynthesis) of these forests was 1380 ± 330 gC m-2 y-1 (mean ±SD). On average, 80% of GPP was respired by autotrophs and heterotrophs and released back into the atmosphere (total ecosystem respiration, TER = 1100 ± 260 gC m-2 y-1 ). Mean annual soil respiration (SR) was 760 ± 340 gC m-2 y-1 (55% of GPP and 69% of TER). Among the investigated forests, large differences were observed in annual SR and TER that were not correlated with mean annual temperature. However, a significant correlation was observed between annual SR and TER and GPP among the relatively undisturbed forests. On the assumption that (i) root respiration is constrained by the allocation of photosynthates to the roots, which is coupled to productivity, and that (ii) the largest fraction of heterotrophic soil respiration originates from decomposition of young organic matter (leaves, fine roots), whose availability also depends on primary productivity, it is hypothesized that differences in SR among forests are likely to depend more on productivity than on temperature. At sites where soil disturbance has occurred (e.g. ploughing, drainage), soil espiration was a larger component of the ecosystem C budget and deviated from the relationship between annual SR (and TER) and GPP observed among the less-disturbed forests. At one particular forest, carbon losses from the soil were so large, that in some years the site became a net source of carbon to the atmosphere. Excluding the disturbed sites from the present analysis reduced mean SR to 660 ± 290 gC m-2 y-1 , representing 49% of GPP and 63% of TER in the relatively undisturbed forest ecosystems. [ABSTRACT FROM AUTHOR]