Ozone Deposition to a Coniferous and Deciduous Forest in the Czech Republic

Estimates of ozone concentration and deposition flux to coniferous and deciduous forest in the Czech Republic on a 1 × 1 km grid during growing season (April–September) of the year 2001 are presented. Ozone deposition flux was derived from ozone concentrations in the atmosphere and from its deposition velocities. To quantify the spatial pattern in surface concentrations at 1 km resolution incorporating topography, empirical methods are used. The procedure maps ozone concentrations from the period of the day when measurements are representative for the forest areas of countryside. The effects of boundary layer stability are quantified using the observed relationship between the diurnal variability of surface ozone concentration and altitude. Ozone deposition velocities were calculated according to a multiple resistance model incorporating aerodynamic resistance (R _a ), laminar layer resistance (R _b ) and surface resistance (R _c ). Surface resistance (R _c ) comprises stomatal resistance (R _sto ). R _sto was calculated with respect to global radiation, surface air temperature and land cover. Modelled total and stomatal ozone fluxes are compared with the maps describing equivalent values of AOT40 (accumulated exposure over threshold of 40 ppb). For forests, the critical level (9,000 ppbh May–July daylight hours) is exceeded over 50% of forested territory. This indicates the potential for effects on large areas of forest. There is significiant correspondence between the exposure index AOT40 and the total ozone flux, but the relation between the total ozone flux and AOT40 exposure index is not clear in all parts of the forest territory.     

Characteristics of an Ozone Deposition Module

An ozone deposition module is being developed to allow the estimation of stomatal fluxes of ozone into a number of vegetation types. This model is designed to be linked into a regional chemical-transport model for use within the European Monitoring and Evaluation Programme (EMEP), to provide information on possible risks to vegetation across Europe. This paper investigates some characteristics of this deposition module, for sites in very different climate zones. The model results suggest that both stomatal and non-stomatal fluxes are comparable in magnitude.     

Validating a New Model for N Sequestration in Forest Soil Organic Matter

A conceptual model for N sequestration into the terrestrial nitrogen(N) sink is presented. The model uses foliar litter-fall data, limit values for litter decomposition, and calculated N concentration at the limit value (N_limit), giving the N concentration in the hypothesized stable remains. The N_limit values were determined extrapolating a linear relationship between accumulated litter mass loss and the increasing litter N concentration to the limit value. Thesequestration rates for N in boreal forest humus were calculated and validated for a Scots pine (Pinus sylvestris L.) monocultural stand and mixed stands with Scots pine, Norway spruce (Picea abies L.), and silver birch (Betula pendula L.). The calculated stable N fraction was compared to actually measured amounts of N in humus layers that started to accumulate 2984, 2081, 1106, and 120 yr BP. Sequestration rates of N were measured to be 0.255, 0.221, 0.147, and 0.168 g m^-2 yr^-1 and modeled to be 0.204, 0.207, 0.190, and 0.190 g m^-2 yr^-1, respectively, with missing fractions being 11.0, 1.5, 30.8, and 13.3%, respectively. The more N-rich the litter, the larger was the N fraction sequestered. This was found for experimental Scots pine needle litter (n = 6) and for 53 decomposition studies, encompassing seven litter species. The amounts of N sequestered annually ranged from ca. 1–2 kg ha^-1 yr^-1 under nutrient-poor boreal conditions to about 30 kgha^-1 yr^-1 in temperate, more nutrient-rich forests.     

Deposition Velocities of SO2 and O3 over Agricultural and Forest Ecosystems

The results of field studies that measured the flux anddeposition velocity of SO₂ and O₃ are reported. Three of the studies were over agricultural crops (pasture, corn, and soybean), and two were over forest (a deciduous forest and a mixed coniferous–deciduous forest). In all cases the deposition velocity for SO₂ was higher than that for O₃. Diurnal cycles of SO₂ deposition velocity were similar in shape, but not magnitude for all surfaces; however those for O₃ showed some difference between forest sites where the peak was in the morning, and the agricultural sites where the peak occurred at mid-day. Seasonal cycles of SO₂ were affected by deposition to surfaces when leaves were not active, yet surface conductance is significant, but not for O₃ where stomatal uptake is the primary pathway for deposition.(On assignment to the National Exposure Research Lab., US EPA) (e-mail:     

Integrated Nitrogen and Flow Modelling (INCA) in a Boreal River Basin Dominated by Forestry: Scenarios of Environmental Change

A new version (v1.7) of the Integrated Nitrogen in CAtchments model(INCA) was applied to the northern boreal Simojoki river basin (3160 km²) in Finland. The INCA model is a semi-distributed, dynamic nitrogen (N) process model which simulates N transport and processes in catchments. The INCA model was applied to model flow and seasonal inorganic N dynamics of the river Simojoki basin over the period 1994–1996, and validated for two more years. Both calibration and validation of the model were successful. The model was able to simulate annual dynamics of inorganic N concentrations in the river. The effects of forest management and atmospheric deposition on inorganic N fluxes to the sea in 2010 were studied. Three scenarios were applied for forestry practices and two for deposition. The effects of forest cutting scenarios and atmospheric deposition scenarios on inorganic N flux to the sea were small. The combination of the maximum technically possible reduction of N deposition and a decrease of 100% in forest cutting and peat mining areas decreased NO₃ ^--N flux by 6.0% and NH₄ ⁺-N flux by 3.1%.     

Ozone Dry Deposition Velocities for Coastal Waters

Air-sea exchange rates for ozone were measured by the eddy correlation technique at a site on the north Norfolk coast in the UK. The average surface resistance to ozone uptake was found to be, r_s(O₃) = 1,000 ± 100 s m^-1. Micrometeorological measurements of trace gas fluxes to ocean surfaces are rare but a review of available measurements suggests that we can constrain sea water surface resistance for ozone to between 1,000 (Regener (1974), and this work) and 1,890 s m^-1 (Lenschow et al., 1982), yielding surface deposition velocities between 0.53 and 1.0 mm s^-1. These values are more than an order of magnitude greater than can be explained by laboratory determined mass accommodation coefficients for ozone to water. The importance of dry deposition with respect to process air-sea exchange models is highlighted. A trend in surface deposition velocity with wind speed was also observed supporting a surface chemical enhancement mechanism of ozone uptake which in turn is enhanced by near surface mixing processes.     

Effects of Soil Moisture Variations on Deposition Velocities Above Vegetation

The parameterized subgrid-scale surface flux (PASS) modelprovides a simplified means of using remote sensing data from satellites and limited surface meteorological information to estimate the influence of soil moisture on bulk canopy stomatalresistances to the uptake of gases over extended areas.PASS-generated estimates of bulk canopy stomatal resistance were usedin a dry deposition module to compute gas deposition velocitieswith a horizontal resolution of 200 m for approximately 5000 km² of agricultural crops and rangeland. Results were compared with measurements of O₃ flux and concentrations made during April and May 1997 at two surface stations and from an aircraft. The trend in simulated O₃ deposition velocityduring soil moisture drydown over a period of a few days matchedthe trend observed at the two surface stations. For areas underthe aircraft flight paths, the variability in simulated O₃ deposition velocity was substantially smaller than the observedvariability, while the averages over tens of kilometers were usually in agreement within 0.1 cm s^-1. Model results indicated that soil moisture can have a major role in depositionof O₃ and other substances strongly affected by canopy stomatal resistance.     

Ozone Deposition at a Forest Site in NE Bavaria

The dry deposition of ozone to aconiferous forest in northeastern Bavaria(southern Germany) was quantified during 1999with both the eddy correlation method and a bigleaf model. The model included parameterizationsof the atmospheric transfer resistances fromdirect measurements, stomatal resistance from aplant ecological model, and an estimation of thecuticle resistance as function of leaf wetness.Early in the season, the measured and themodelled deposition fluxes were in goodagreement, although the modelled fluxes tended tounderestimate the measured ones. Thisunderestimation was more pronounced in the latesummer, when high nocturnal fluxes werefrequently measured. The model parameterizationof the cuticle and the stomatal resistances didnot allow for such high fluxes. In these cases,the 24 hour average of the measured fluxes wereup to 4.5 times higher than the modelled ones.The reasons for these large discrepancies remainunknown. However, assigning the unaccounted partof the deposition to a nonstomatal surfacedeposition pathway, a new parameterization of therespective resistance yielded an average value of300 s m^-1. It exhibited a decreasing trendthrough the vegetation period.     

A Coupled Land-Surface and Dry Deposition Model and Comparison to Field Measurements of Surface Heat,Moisture, and Ozone Fluxes

We have developed a coupled land-surface and drydeposition model for realistic treatment of surface fluxes ofheat, moisture, and chemical dry deposition within acomprehensive air quality modelling system. A new land-surfacemodel (LSM) with explicit treatment of soil moisture andevapotranspiration and an indirect soil moisture nudging schemehas been added to a mesoscale meteorology model. The new drydeposition model uses the same aerodynamic and bulk stomatalresistances computed for evapotranspiration in the LSM. Thisprovides consistent land-surface and boundary layer propertiesacross the meteorological and chemical components of the system. The coupled dry deposition model also has the advantage of beingable to respond to changing soil moisture and vegetationconditions. Modelled surface fluxes of sensible and latent heatas well as ozone dry deposition velocities were compared to twofield experiments: a soybean field in Kentucky during summer 1995and a mixed forest in the Adirondacks of New York in July 1998.(on assignment to the National Exposure Research Laboratory, U.S. Environmental Protection Agency) (author for correspondence, e-mail(on assignment to the National Exposure Research Laboratory, U.S. Environmental Protection Agency)     

Direct and Indirect Effects of Soil Pollution by Lignite Mining

Lignite mining and processing has caused a pronounced impact both directly and indirectly on soils and ecosystems across large areas of the former GDR. We studied soils of pine forest ecosystems at sites affected by severe alkaline dust and sulphur deposition, stemming from lignite fired power plant emission, and at dumped sites from lignite mining. In this paper we summarize our main results and evaluate the long-term impact of lignite mining and combustion on the environment. The pine ecosystems on naturally developed soils show a clear effect of deposition history along a former deposition gradient with distinct changes in chemical properties of organic surface layers and mineral soil as well as in element turnover and cycling rates. Afforested sites on mining dumps are directly affected by the composition of the dumped substrates. Over a large area (800 km²) these substrates are dominated by Tertiary sediments with varying amounts of lignitic particles and pyrite that result in phytotoxic site conditions (pH < 3, high salt and metal contents). High amelioration doses of liming material (up to 200 t ha⁻¹) were applied for restoration purposes. We studied the development of these sites over a period of 60 years using a false-time series approach. Beside the extreme soil conditions, element budgets of these sites are characterized by very high element release rates over decades caused by pyrite oxidation and primary mineral weathering.     

CHEMIFOG_V – A Model to Simulate Radiation Fogs and their Interaction with Vegetation and Chemistry

Radiation fog is an important modifier of atmosphericcompounds in the planetary boundary layer. In vegetated areas effects are especially pronounced due to the enlarged surface area. Besides affectingthe lower boundary of atmospheric models fog acts as amulti-phase reaction chamber leading to acid deposition. Here we present the 1-dimensional radiation fog modelCHEMIFOG_V to simulate regional radiation fogevents. The key feature of the fog model is thedetailed microphysics, where the aerosol/dropletspectrum is describedwith a joint 2-dimensional distribution, but also thedynamics, thermodynamics, and radiative transfer are calculated. Toinvestigate the interaction between fog and the biosphere amulti-layer vegetation module, including a soil module as well as a drydeposition module were coupled. Vegetation influences thedynamics, thermodynamics, and the radiation field of the lowestatmospheric layers. With CHEMIFOG_V, numerical case studieson dry and moist deposition processes on vegetation surfaces wereperformed. Hereby multi-phase chemistry and the processing of aerosolswere considered. The results show that the chemical composition of thedeposited fog droplets is mainly determined by the aerosol composition. Dry deposition fluxes are dependent on the incoming radiation and the leaves' surface conditions with respect to water coverage.Due to chemical aerosol processing and deposition, the aerosol spectrumis significantly modified in the planetary boundary layer.     

Deposition and Storage of Spheroidal Carbonaceous Fly-Ash Particles in European Mountain Lake Sediments and Catchment Soils

Spheroidal carbonaceous particles(SCPs) are produced only from high temperaturecombustion of fossil-fuels. In mountain lakesystems, they provide an unambiguous indicator ofatmospheric deposition. In order to comparedepositional fluxes of SCPs between mountainareas experiencing various pollutant regimes,intensive bulk deposition sampling was undertakenat five sites across Europe. Catchment soil coresand lake sediment cores were also taken at eachsite to compare SCP storage over the post-industrial period. Atmospheric, sediment and soilSCP data showed similar patterns. Highestcontamination was found in Scotland, Slovakia andSpain with the Austrian site intermediate and themid-Norwegian site least contaminated. A highproportion of accumulated SCPs were found to bestored in catchment soils at each site.Therefore, a significant increase in soilerosion, possibly as a result of future climatechange, could lead to the input of largequantities of catchment stored SCPs and, byimplication, other atmospherically depositedcontaminants to the lake ecosystem.     

Mercury and Methylmercury in Runoff from a Forested Catchment – Concentrations, Fluxes, and Their Response to Manipulations

Measurements of TotHg (total mercury) and MeHg (methylmercury) in runoff from the covered catchment G1 and the reference catchment F1 at Lake Gårdsjön, Sweden, have been performed and evaluated. The roof over the covered catchment limits atmospheric deposition input of TotHg and MeHg and a response in runoff concentrations and transport was expected. Based on data from 10 yr of monitoring, no statistically significant change in runoff flux of TotHg or MeHg can be observed. A slight decrease in MeHg output in the covered catchment was observed after 2 yr of the experiment. This can be explained as a temporary effect caused by the roof construction. The main conclusion is that release of TotHg and MeHg from the forest soil is controlled by factors other that wet deposition input, for example the mineralisation of organic matter. Furthermore, there is no indication of a depletion of the Hg pool in the soil. In spring 1999, the reference catchment F1 was affected by forestry machinery significantly disturbing the forest soil layer in a limited area. This caused MeHg concentrations to increase dramatically in runoff and led to an increase of the annual transport by at least a factor of 3. This indicates that forestry and other activities that disturb forest soils may be important for controlling MeHg fluxes to aquatic ecosystems.     

The Role of Cloud Processing in the Relationship Between Wet Deposited Sulphur and Sulphur Dioxide Emissions

It is well established that wet deposition of sulphate in the UKhas fallen by a much smaller fraction than have emissions of sulphur dioxide. Dry deposition of sulphur has decreased in proportion to the decline in emissions. A number of suggestionshave been made which offer possible explanations for this non-linearity between emissions and wet deposition. In this paper amodel of the processing of sulphur dioxide by aqueous phase cloudchemistry in a cloudy boundary layer is presented. This work doesnot simulate all the details of the mechanisms by which sulphate is incorporated into precipitation. It does, however, explorethe non-linearity of this oxidation process. It is shown that theoxidation of sulphur dioxide, in these conditions, over the UK isdominated by oxidation by ozone. The rate of sulphate productionis then controlled by the availability of the one basic trace gasin the atmosphere ammonia. Using realistic concentrations of thereacting species this is found to simulate well the observed non-linearity. The model predicts that sulphate and sulphur dioxideconcentrations will be uncorrelated in the cloudy boundary layerbut that ammonium and sulphate will be well correlated. Fieldobservations at a cloudy site in Northern England are consistentwith these predictions.     

Evaluation and Improvement of a Dry Deposition Model using SO2 and O3 Measurements over a Mixed Forest

A dry deposition model (RDM) for operational application has beenevaluated and modified in the present study. Field measurements of friction velocity and dry deposition velocity of SO₂ andO₃ over a mixed forest have been used to evaluate RDM. It was found that RDM predicts friction velocities very close to measurements and thus it can predict reasonable aerodynamic resistance. RDM overestimated O₃ deposition during dry nighttime conditions and underestimated both O₃ andSO₂deposition for early morning hours. It could not predict the mean diurnal variation in deposition velocity for either O₃ or SO₂ deposition under wet surface conditions. Modifications have been made for O₃ and SO₂ dry deposition based on the comparison of results and based upon additional published data. Compared to an earlier version of RDM, the modified versionpredicts better results for O₃ and SO₂ dry deposition,especially under rain and dew conditions.     

Using Meteorological Model Output as a Surrogate for On-Site Observations to Predict Deposition Velocity

The National Oceanic and Atmospheric Administration's Multi-Layer Model (NOAA-MLM) is used by several operational dry deposition networks for estimating the deposition velocity of O₃, SO₂, HNO₃, and particles. The NOAA-MLM requires hourly values of meteorological variables. Since collection of on-site meteorology can be expensive, a study was performed to compare NOAA-MLM predicted deposition velocitiesusing modeled meteorological data in lieu of on-site meteorological data. NOAA-MLM was run for three sites in the Clean Air Status and Trends Network using on-site data as well as the output of two mesoscale meteorological models, Eta and MM5. The differences between the deposition velocities predictedusing the mesoscale models and those predicted using the on-sitemeteorological measurements ranged from –0.001 to 0.106 cm s^-1 and were within the model error determined in NOAA-MLM evaluation studies. This research shows that the NOAA-MLM is particularly sensitive to differences in atmospheric turbulence,soil moisture budget, and canopy wetness.(On assignment to the National Exposure Research Laboratory, U.S. Environmental Protection Agency, Research Triangle Park, North Carolina.) (author for correspondence, e-mail     

An Analysis of the Structure of the Simple Mass Balance Equation: Implications for Testing National Critical Loads Maps

The critical loads concept is used by the UN-ECEConvention on Long Range Transboundary Air Pollution(CLRTAP) for setting pollution reduction targets.Increasing numbers of countries are adopting the SimpleMass Balance equation (SMB) to calculate critical loads ofacidifying S and N for forest soils. The equation is madeup of a series of mass balances each of which is used tocalculate a leaching flux. The assumptions in the SMBequation were investigated by testing its ability topredict current sulphur load and by comparing each of thecalculated leaching fluxes to measured rates. It was notpossible to predict current sulphur load at our sites usingthe SMB equation. The leaching tests demonstrated that,primarily due to its steady state assumptions, the SMBequation generates critical loads that are theoretical longterm estimates of risk, and are untestable. Thesimplifying assumptions sometimes lead to illogicalresults. Some of these can be improved by adding a final,simple but dynamic, calculation step to determine theexpected time until effects are observed. Theacceptability of combining annual average data, which bestapproximates steady state, with a biological indicator isquestionable. It is not possible to test critical loadscalculated using the SMB equation when applied with all ofits assumptions but it is possible to test its fundamentalapproach using non steady state data.     

Deposition Loads of Sulphur and Nitrogen in Germany

High spatial resolution maps of deposition loads in Germanyare produced as an input for abatement strategy research andfor critical loads exceedance calculations on a nationalscale. In this paper methods ofmapping total deposition loads in Germany and preliminarymaps of nitrogen and sulphur deposition loads for the year1993 are presented. A comparison of these mapping resultswith EMEP deposition mapping results has been carried out.The differences in the results of the German national and theEuropean EMEP mapping, due to different databases anddifferent methods, are quantified and discussed. Highresolution maps of deposition loads are compared to Europeanlow resolution maps on the same temporal and spatial scale,assuming that on average both should lead to similar results.However, the average differencescalculated for 23 EMEP 150 × 150 km² grid cells over Germanywere found to be 33% higher for sulphur (S) total depositionby the German method 65% higher for S dry deposition and1% lower for S wet deposition. The German results fornitrogen (N) total deposition are 2% higher than the EMEPresult 22% higher for N dry deposition and 10% lower for Nwet deposition.     

Growth and Nitrogen Availability of Red Pine Seedlings under High Nitrogen Load and Elevated Ozone

To evaluate the effect of increasing nitrogen (N) deposition and tropospheric ozone (O₃) concentrations on N-saturated forest ecosystems, we investigated the response of Japanese red pine (Pinus densiflora), an N-saturation sensitive tree species, to increasing N load under elevated O₃ concentrations. One-year-old seedlings of red pine were treated with three levels of N supply (0, 50 and 100 mg N L^-1 fresh soil volume) under two levels of atmospheric O₃ concentration (< 5 and 60 ppb) for two growing seasons. Nitrogen treatment did not stimulate dry matter production of the seedlings. Growth inhibition was observed in the highest N treatment under low O₃ and in the two higher N treatments under elevated O₃. Irrespective of the O₃ concentration, increasing N supply negatively affected root growth and mycorrhizal development in fine roots, resulting in a reduction in P and Mg uptake from the soil. Net photosynthetic rate was significantly reduced by both the highest N treatment under low O₃ and the two higher N treatments under elevated O₃, together with decreased N-availability to Rubisco. Nitrogen assimilated from NO₃ ^- to amino acid in the needles was not affected by the treatments. However, needle protein concentration was reduced by the highest N-treatment under low O₃ and by the two higher N-treatments under elevated O₃. These results suggest that elevated O₃ potentially disturbs the N-availability in the form of protein including Rubisco, and may advance the negative effects of excessive N-deposition on N-sensitive plant species in N-saturated forests.