Quantifying simultaneous fluxes of ozone, carbon dioxide and water vapor above a subalpine forest ecosystem

Assessing the long-term exchange of trace gases and energy between terrestrial ecosystems and the atmosphere is an important priority of the current climate change research. In this regard, it is particularly significant to provide valid data on simultaneous fluxes of carbon, water vapor and pollutants over representative ecosystems. Eddy covariance measurements and model analyses of such combined fluxes over a subalpine coniferous forest in southern Wyoming (USA) are presented. While the exchange of water vapor and ozone are successfully measured by the eddy covariance system, fluxes of carbon dioxide (CO(2)) are uncertain. This is established by comparing measured fluxes with simulations produced by a detailed biophysical model (FORFLUX). The bias in CO(2) flux measurements is partially attributed to below-canopy advection caused by a complex terrain. We emphasize the difficulty of obtaining continuous long-term flux data in mountainous areas by direct measurements. Instrumental records are combined with simulation models as a feasible approach to assess seasonal and annual ecosystem exchange of carbon, water and ozone in alpine environments. The viability of this approach is demonstrated by: (1) showing the ability of the FORFLUX model to predict observed fluxes over a 9-day period in the summer of 1996; and (2) applying the model to estimate seasonal dynamics and annual totals of ozone deposition and carbon, and water vapor exchange at our study site. Estimated fluxes above this subalpine ecosystem in 1996 are: 195 g C m(-2) year(-1) net ecosystem production, 277 g C m(-2) year(-1) net primary production, 535 mm year(-1) total evapo-transpiration, 174 mm year(-1) canopy transpiration, 2.9 g m(-2) year(-1) total ozone deposition, and 1.72 g O(3) m(-2) year(-1) plant ozone uptake via leaf stomata. Given the large portion of non-stomatal ozone uptake (i.e. 41% of the total annual flux) predicted for this site, we suggest that future research of pollution-vegetation interactions should relate plant response to actively assimilated ozone by foliage rather than to total deposition. In this regard, we propose the Physiological Ozone Uptake Per Unit of Leaf Area (POUPULA) as a practical index for quantifying vegetation vulnerability to ozone damage. We estimate POUPULA to be 0.614 g O(3) m(-2) leaf area year(-1) at our subalpine site in 1996.     

Modeling above-canopy CO2 flux and evapotranspiration in wheat

Simulations of above-canopy water vapor and CO2 fluxes were calculated by the USGF linked model of canopy gas exchange and subsurface processes for the 1996-1997 winter wheat season at the AmeriFlux Wheat Site, Oklahoma. Soil surface CO2 flux plus canopy gas exchange and transpiration plus soil evaporation modeled the CO2 and water vapor fluxes, respectively. Parameter values for net photosynthesis, respiration and transpiration were obtained from published sources, generated from Wheat Site data, or estimated by minimizing standard deviation between model and data. The mean measured downward flux of CO2 during rapid growth and maturity of the crop was -0.45 mg m(-2) s(-1) compared to simulated flux of -0.47. Simulated downward CO2 flux exceeded measured values during rapid growth of the crop but underestimated the flux during maturity. For the entire 285-day period, the mean measured upward CO2 flux at night was 0.06 and simulated flux was 0.05.     

Surface flux measurements of CO2 and N2O from a dried rice paddy in Japan during a fallow winter season

The CO2 and N2O soil emissions at a rice paddy in Mase, Japan, were measured by enclosures during a fallow winter season. The Mase site, one of the AsiaFlux Network sites in Japan, has been monitored for moisture, heat, and CO2 fluxes since August 1999. The paddy soil was found to be a source of both CO2 and N2O flux from this experiment. The CO2 and N2O fluxes ranged from -27.6 to 160.4 microg CO2/m2/sec (average of 49.1 +/- 42.7 microg CO2/m2/sec) and from -4.4 to 129.5 ng N2O/m2/sec (average of 40.3 +/- 35.6 ng N2O/m2/ sec), respectively. A bimodal trend, which has a sub-peak in the morning around 10:00 a.m. and a primary peak between 2:00 and 3:00 p.m., was observed. Gas fluxes increased with soil temperature, but this temperature dependency seemed to occur only on the calm days. Average CO2 and N2O fluxes were 27.7 microg CO2/m2/sec and 13.4 ng N2O/m2/sec, with relatively small fluctuation during windy days, while averages of 69.3 microg CO2/m2/sec and 65.8 ng N2O/m2/sec were measured during calm days. This relationship was thought to be a result of strong surface winds, which enhance gas exchange between the soil surface and the atmosphere, thus reducing the gas emissions from soil surfaces.     

Influence of livestock grazing on C sequestration in semi-arid mixed-grass and short-grass rangelands

We evaluated the effects of livestock grazing on C content of the plant-soil system (to 60 cm) of two semi-arid grasslands: a mixed-grass prairie (grazed 12 years), and a short-grass steppe (grazed 56 years). Grazing treatments included season-long grazing at heavy and light stocking rates, and non-grazed exclosures. Significantly higher soil C (0-30cm) was measured in grazed pastures compared to non-grazed exclosures, although for the short-grass steppe higher soil C was observed with the heavy grazing treatment only. Excluding grazing caused an immobilization of C in excessive aboveground plant litter, and an increase in annual forbs and grasses which lack dense fibrous rooting systems conducive to soil organic matter formation and accumulation. Our data indicate that higher soil C with grazing was in part the result of more rapid annual shoot turnover, and redistribution of C within the plant-soil system as a result of changes in plant species composition.     

Aspect differences in above- and belowground carbon allocation: a Montana case-study

Aboveground net primary production (ANPP) and belowground gross primary production (BGPP) of all vegetation were measured in eight young, paired plots on a north and south aspect in western Montana. Stands of high and low overstory tree leaf area index (LAI) were compared. BGPP increased with ANPP, though they were not directly proportional. ANPP ranged from 1550 to 4400 kg C ha(-1) year(-1) and BGPP ranged from 1360 to 3500 kg C ha(-1) year(-1). ANPP and BGPP were both significantly related to LAI and aspect, where both were greater on the north aspect at any given LAI. Litterfall represented the largest share of ANPP; increases in overstory biomass represented the next largest share. Soil CO2 flux was higher on the north aspect. We conclude that growth differences were not simply a matter of re-allocating carbon between root production and ANPP. Rather, both production and allocation were different among the sites.     

Effects of environmental factors on N2O emission from and CH4 uptake by the typical grasslands in the Inner Mongolia

The fluxes of N2O emission from and CH4 uptake by the typical semi-arid grasslands in the Inner Mongolia, China were measured in 1998-1999. Three steppes, i.e. the ungrazed Leymus chinensis (LC), the moderately grazed Leymus chinensis (LC) and the ungrazed Stipa grandis (SG), were investigated, at a measurement frequency of once per week in the growing seasons and once per month in the non-growing seasons of the LC steppes. In addition, four diurnal-cycles of the growing seasons of the LC steppes, each in an individual stage of grass growth, were measured. The investigated steppes play a role of source for the atmospheric N2O and sink for the atmospheric CH4, with a N2O emission flux of 0.06-0.21 kg N ha(-1) yr(-1) and a CH4 uptake flux of 1.8-2.3 kg C ha(-1) yr(-1). Soil moisture primarily and positively regulates the spatial and seasonal variability of N2O emission. The usual difference in soil moisture among various semi-arid steppes does not lead to significantly different CH4 uptake intensities. Soil moisture, however, negatively regulates the seasonal variability in CH4 uptake. Soil temperature of the most top layer might be the primary driving factor for CH4 uptake when soil moisture is relatively low. The annual net emission of N2O and CH4 from the ungrazed LC steppe, the moderately grazed LC steppe and the ungrazed SG steppe is at a CO2 equivalent rate of 7.7, 0.8 and -7.5 kg CO2-C ha(-1) yr(-1), respectively, which is at an ignorable level. This implies that the role of the semi-arid grasslands in the atmospheric greenhouse effect in terms of net emission of greenhouse gases (CO2, CH4 and N2O) may exclusively depend upon the net exchange of net ecosystem CO2 exchange.     

Evaluation of use of EcoCELL technology for quantifying total gaseous mercury fluxes over background substrates

Total gaseous mercury (Hg) fluxes from large (7.3×5.5×4.5 m, L×W×D) climate-controlled gas exchange mesocosms (Ecologically Controlled Enclosed Lysimeter Laboratories or EcoCELLs) containing tallgrass prairie soil–plant monoliths were measured from 2002 to 2005. EcoCELL Hg fluxes (calculated based on the difference in air Hg concentrations inside mesocosms and in incoming air, soil area of the monoliths, and airflow through the system) indicated a net annual emission of 102 μg m⁻², while soil Hg fluxes measured simultaneously using a dynamic flux chamber were an order of magnitude lower. Since Hg fluxes measured from empty EcoCELLs in winter and when housing the soil–plant monoliths at the same time of year were similar, we hypothesized that the Hg signal generated by the tallgrass prairie soil–plant monoliths was too low to be detected using the EcoCELL technology. Because mesocosm Hg exchange was correlated with solar radiation and temperature, with the largest emissions occurring at midday and in the summer, we also hypothesized that the flux from mesocosm infrastructure would change over time. Limited by the ongoing experiment, the EcoCELLs were manipulated to test the above hypotheses. When monoliths were completely covered and excluded from the exchange with the surrounding air, mesocosm Hg exchange was unaffected. Furthermore, removal of vegetation at the end of each growing season did not affect mesocosm Hg fluxes. Tests with changing mesocosm airflow also indicated that the signal from the tallgrass prairie monoliths was not being measured. These results suggest that, although EcoCELLs performed well in a study using Hg contaminated soils and have been successfully applied to understand processes controlling Hg fluxes, there are limitations of this technology for quantifying Hg exchange from background substrates. Prior to the use of similar systems the detection limit and Hg exchange from an empty system need to be carefully quantified.     

Regional estimation of current and future forest biomass

The 90,674 wildland fires that burned 2.9 million ha at an estimated suppression cost of $1.6 billion in the United States during the 2000 fire season demonstrated that forest fuel loading has become a hazard to life, property, and ecosystem health as a result of past fire exclusion policies and practices. The fire regime at any given location in these regions is a result of complex interactions between forest biomass, topography, ignitions, and weather. Forest structure and biomass are important aspects in determining current and future fire regimes. Efforts to quantify live and dead forest biomass at the local to regional scale has been hindered by the uncertainty surrounding the measurement and modeling of forest ecosystem processes and fluxes. The interaction of elevated CO2 with climate, soil nutrients, and other forest management factors that affect forest growth and fuel loading will play a major role in determining future forest stand growth and the distribution of species across the southern United States. The use of satellite image analysis has been tested for timely and accurate measurement of spatially explicit land use change and is well suited for use in inventory and monitoring of forest carbon. The incorporation of Landsat Thematic Mapper data coupled with a physiologically based productivity model (PnET), soil water holding capacity, and historic and projected climatic data provides an opportunity to enhance field plot based forest inventory and monitoring methodologies. We use periodic forest inventory data from the USDA Forest Service's Forest Inventory and Analysis (FIA) project to obtain estimates of forest area and type to generate estimates of carbon storage for evergreen, deciduous, and mixed forest classes for use in an assessment of remotely sensed forest cover at the regional scale for the southern United States. The displays of net primary productivity (NPP) generated from the PnET model show areas of high and low forest carbon storage potential and their spatial relationship to other landscape features for the southern United States. At the regional scale, predicted annual NPP in 1992 ranged from 836 to 2181 g/m2/year for evergreen forests and 769-2634 g/m2/year for deciduous forests with a regional mean for all forest land of 1448 g/m2/year. Prediction of annual NPP in 2050 ranged from 913 to 2076 g/m2/year for evergreen forest types to 1214-2376 g/m2/year for deciduous forest types with a regional mean for all forest land of 1659 g/m2/year. The changes in forest productivity from 1992 to 2050 are shown to display potential areas of increased or decreased forest biomass. This methodology addresses the need for spatially quantifying forest carbon in the terrestrial biosphere to assess forest productivity and wildland fire fuels.     

Monitoring the multi-year carbon balance of a subarctic palsa mire with micrometeorological techniques

This article reports a dataset on 8 years of monitoring carbon fluxes in a subarctic palsa mire based on micrometeorological eddy covariance measurements. The mire is a complex with wet minerotrophic areas and elevated dry palsa as well as intermediate sub-ecosystems. The measurements document primarily the emission originating from the wet parts of the mire dominated by a rather homogenous cover of Eriophorum angustifolium. The CO(2)/CH(4) flux measurements performed during the years 2001-2008 showed that the areas represented in the measurements were a relatively stable sink of carbon with an average annual rate of uptake amounting to on average -46 g C m(-2) y(-1) including an equally stable loss through CH(4) emissions (18-22 g CH(4)-C m(-2) y(-1)). This consistent carbon sink combined with substantial CH(4) emissions is most likely what is to be expected as the permafrost under palsa mires degrades in response to climate warming.     

Growth, phenology and reproduction of an arid-environment winter ephemeral Dimorphotheca pluvialis in response to combined increases in CO2 and UV-B radiation

The winter ephemeral Dimorphotheca pluvialis was grown in open-top chambers in ambient or elevated CO2 (350 or 650 micromol mol(-1)), combined with ambient (2.39 to 7.59 kJ m(-2) d(-1)) or increased (4.94 to 11.13 kJ m(-2) d(-1)) UV-B radiation. Net CO2 assimilation rate and leaf water use efficiency increased in elevated CO2, but increased UV-B did not affect gas exchange. Leaf biomass was greater under increased UV-B, but vegetative biomass was unaffected in elevated CO2. Initiation of reproduction was delayed, and proportional investment in reproductive biomass at harvest was reduced in elevated CO2. Increased UV-B stimulated reproduction, particularly in ambient CO2, but also in elevated CO2 at a later stage. Changes in reproductive phenology and prolonged development in elevated CO2 during the stressful late season could indirectly be detrimental to reproductive success of D. pluvialis, but stimulation of reproduction by enhanced UV-B may to some extent mitigate this.     

Removal of methyl chloroform in a coastal salt marsh of eastern China

The atmospheric burden of methyl chloroform (CH(3)CCl(3)) is still considerable due to its long atmospheric lifetime, although CH(3)CCl(3) emissions have declined considerably since it was included into the Montreal Protocol. Moreover, CH(3)CCl(3) emissions are used to estimate hydroxyl radical (OH) levels, trends, and hemispheric distributions, and thus the mass balance of the trace gas in the atmosphere is critical for characterizing OH concentrations. Salt marshes may be a potential sink for CH(3)CCl(3) due to its anoxic environment and abundant organic matter in sediments. In this study, seasonal dynamics of CH(3)CCl(3) fluxes were measured using static flux chambers from April 2004 to January 2005, along an elevational gradient of a coastal salt marsh in eastern China. To estimate the contribution of higher plants to the gas flux, plant aboveground biomass was experimentally harvested and the flux difference between the treatment and the intact was examined. In addition, the flux was analyzed in relation to soil and weather conditions. Along the elevational gradient, the salt marsh generally acted as a net sink of CH(3)CCl(3) in the growing season (from April to October). The flux of CH(3)CCl(3) ranged between -3.38 and -32.03 nmol m(-2)d(-1) (positive for emission and negative for consumption), and the maximum negative rate occurred at the cordgrass marsh. However, the measurements made during inundation indicated that the mudflat was a net source of CH(3)CCl(3). In the non-growing season (from November to March), the vegetated marsh was a minor source of CH(3)CCl(3) when soil was frozen, the emission rate ranging from 3.43 to 7.77 nmol m(-2)d(-1). However, the mudflat was a minor sink of CH(3)CCl(3) whether it was frozen or not in the non-growing season. Overall, the coastal salt marsh in eastern China was a large sink for the gas, because the magnitude of consumption rate was lager than that of emission, and because the duration of the growing season was longer than that of the non-growing season. Plant aboveground biomass had a great effect on the flux. Comparative analysis showed that the direction and magnitude of the effect of higher plants on the flux of CH(3)CCl(3) depended on timing of sampling vegetation type. In the growing season the plant biomass decreased the gas flux and acted as a large sink of the gas, whereas it presented as a minor source in the non-growing season. However, the mechanism underlying plant uptake process is not clear. The CH(3)CCl(3) flux was positively related to the dissolved salt concentration and organic matter content in soil, as well as light intensity, but it was negatively related to soil temperature, sulfate concentrations, and initial ambient atmospheric concentrations of CH(3)CCl(3). Our observations have important implications for estimation of the tropospheric lifetime of CH(3)CCl(3) and global OH concentration from the global budget concentration of CH(3)CCl(3).     

Atmospheric deposition of polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans, and dioxin-like polychlorinated biphenyls in the Kanto Region, Japan

The atmospheric bulk (dry and wet) deposition of dioxins was investigated at four locations (Tokyo, Yokohama, Tsukuba, and Tanzawa) in the Kanto region (in Japan) over one year using a stainless-steel pot. Annual average polychlorinated dibenzo-p-dioxins/polychlorinated dibenzofurans (PCDD/PCDF) deposition fluxes were estimated to be from 450 to 1300 ng/m2/yr, and the annual average TEQ fluxes from 5.7 to 17 ng-TEQ/m2/yr at the four locations. The PCDD/PCDF deposition flux was higher in winter than in summer. The deposition flux could be related to ambient temperature, particularly for less chlorinated PCDDs/PCDFs, while the deposition flux is not necessarily related to the amount of precipitation. The PCDD/PCDF deposition flux increased as the particle deposition flux increased, for the winter samples. Based on the ratio of the PCDD/PCDF deposition fluxes to the particle deposition fluxes, the contribution of the reentrainment of soil particles to the TEQ of PCDD/PCDF deposition was considered to be negligible in this region. Based on the air concentrations monitored near our deposition sampling points by the municipalities, the ratio of the annual deposition flux to the annual average air concentration was roughly estimated to be 0.082 cm/s. The range of deposition flux in the Kanto region was estimated to be from 1.5 to 31 (median: 9.8) ng-TEQ/m2/yr based on the range of air concentration data measured by the municipalities. The total annual deposition flux in the entire Kanto region was estimated to range from 50 to 900 g-TEQ/yr (median 320 g-TEQ/yr). This estimated flux was of the same order as the sum of estimated emissions from municipal solid waste incinerators and industrial waste incinerators in the Kanto region. The contributions of dioxin-like PCBs in Yokohama, Tsukuba, and Tanzawa depositions were less than 10% of the total TEQ; however, in Tokyo it was almost equal to or more than 50%.     

Methane production and consumption in an active volcanic environment of Southern Italy

Methane fluxes were measured, using closed chambers, in the Crater of Solfatara volcano, Campi Flegrei (Southern Italy), along eight transects covering areas of the crater presenting different landscape physiognomies. These included open bare areas, presenting high geothermal fluxes, and areas covered by vegetation, which developed along a gradient from the central open area outwards, in the form of maquis, grassland and woodland. Methane fluxes decreased logarithmically (from 150 to -4.5 mg CH4 m(-2)day(-1)) going from the central part of the crater (fangaia) to the forested edges, similarly to the CO2 fluxes (from 1500 g CO2 m(-2)day(-1) in the centre of the crater to almost zero flux in the woodlands). In areas characterized by high emissions, soil presented elevated temperature (up to 70 degrees C at 0-10 cm depth) and extremely low pH (down to 1.8). Conversely, in woodland areas pH was higher (between 3.7 and 5.1) and soil temperature close to air values. Soil (0-10 cm) was sampled, in two different occasions, along the eight transects, and was tested for methane oxidation capacity in laboratory. Areas covered by vegetation mostly consumed CH4 in the following order woodland>macchia>grassland. Methanotrophic activity was also measured in soil from the open bare area. Oxidation rates were comparable to those measured in the plant covered areas and were significantly correlated with field CH4 emissions. The biological mechanism of uptake was demonstrated by the absence of activity in autoclaved replicates. Thus results suggest the existence of a population of micro-organisms adapted to this extreme environment, which are able to oxidize CH4 and whose activity could be stimulated and supported by elevated concentrations of CH4.     

Fluxes of carbon dioxide, methane and nitrous oxide in two contrastive fringing zones of coastal lagoon, Lake Nakaumi, Japan

We measured fluxes of carbon dioxide (CO(2)), methane (CH(4)), and nitrous oxide (N(2)O) simultaneously in two typical fringing zones, sandy shore and salt marsh, of coastal lagoon, Lake Nakaumi, Japan, in mid-summer 2003. Our aim was to quantify net the greenhouse gases (GHGs) fluxes and examine key factors, which control variation of the GHGs fluxes in the two sites. Net CO(2) and CH(4) fluxes were markedly different between the two sites; magnitudes and variations of the both fluxes in sandy shore were lower than those of salt marsh. Meanwhile, magnitude and variation of net N(2)O flux in the two sites were similar. In sandy shore, temporal and spatial variation of the three GHGs fluxes were highly controlled by water level fluctuation derived from astronomic tide. In salt marsh, spatial variation of the three GHGs fluxes were correlated with aboveground biomass, and temporal variation of CO(2) and CH(4) fluxes were correlated with soil temperature. The sum of global warming potential, which was roughly estimated using the observed GHGs fluxes, was ca. 174-fold higher in salt marsh than in sandy shore.     

Methane emission from fields with differences in nitrogen fertilizers and rice varieties in Taiwan paddy soils

Flooded rice fields are one of the major biogenic methane sources. In this study, methane emission rates were measured after transplanting in paddy fields with application of two kinds of nitrogen fertilizers (ammonium sulfate, NH4+-N and potassium nitrate, NO3(-)-N) and with two kinds of rice varieties (Japonica and Indica). The experiment was conducted in fields located at Tainan District Agricultural Improvement Station in Chia-Yi county (23 degrees 25'08"N, 120 degrees 16'26"E) of southern Taiwan throughout the first and the second crop seasons in 1999. The seasonal methane flux in the first crop season with NH4+-N and NO3(-)-N ranged from 2.48 to 2.78 and from 8.65 to 9.22 g CH4 m(-2); and the values ranged 24.6-34.2 and 36.4-52.6 g CH4 m(-2) in the second crop season, respectively. In the first crop season, there were significantly increased 3.1-3.7-fold in methane emission fluxes due to plantation of Indica rice. In comparison of two rice varieties, the Indica rice variety showed a tendency for larger methane emission than the Japonica rice variety in the second crop season. Moreover, ammonium sulfate treatment significantly reduced CH4 emissions by 37-85% emissions compared to potassium nitrate plots. It was concluded that the CH4 emission was markedly dependent on the type of nitrogen fertilizer and rice variety in Taiwan paddy soils.     

Mercury mobility in a salt marsh colonised by Halimione portulacoides

The present study intends to increase the knowledge on the mobility of mercury in a salt marsh colonised by Halimione portulacoides. Mercury distribution in the sediment layers and its incorporation into the plant biomass were assessed, as well as the potential export of mercury from the contaminated area to the adjacent environment. Mercury pools in the sediments ranged from 560 to 943 mg m(-2) and are largely associated with the solid fraction, with just a small amount being associated with the pore waters. Estimated diffusive fluxes of reactive mercury ranged from 1.3 to 103 ng m(-2) d(-1). Despite the above ground biomass values being comparatively higher than below ground biomass values, the mercury pools were much higher in the root system (0.06-0.16 mg m(-2) and 29-102 mg m(-2), respectively). The annual bioaccumulation of mercury in above ground tissues was estimated in 0.11 mg m(-2) y(-1), while in below ground biomass the values were higher (7 2mg m(-2) y(-1)). The turnover rates of H. portulacoides biomass suggest higher mercury mobility within the plant rhizosphere. Taking into account the pools of mercury in above ground biomass, the export of mercury by macro-detritus following the "outwelling hypothesis" is not significant for the mercury balance in the studied ecosystem. The mercury accumulated in the below ground part of the plant is quite mobile, being able to return to the sediment pool throughout the mineralisation process.     

Seasonal air-water exchange fluxes of polychlorinated biphenyls in the Hudson River Estuary

Polychlorinated biphenyls (PCBs) were measured in the air and water over the Hudson River Estuary during six intensive field campaigns from December 1999 to April 2001. Over-water gas-phase SigmaPCB concentrations averaged 1100 pg/m3 and varied with temperature. Dissolved-phase SigmaPCB concentrations averaged 1100 pg/L and displayed no seasonal trend. Uncertainty analysis of the results suggests that PCBs with 5 or fewer chlorines exhibited net volatilization. The direction of net air/water exchange could not be determined for PCBs with 6 or more chlorines. Instantaneous net fluxes of SigmaPCBs ranged from +0.2 to +630 ng m(-2) d(-1). Annual fluxes of SigmaPCBs were predicted from modeled gas-phase concentrations, measured dissolved-phase concentrations, daily surface water temperatures and wind speeds. The net volatilization flux was +62 microg m(-2) yr(-1), corresponding to an annual loss of +28 kg/yr of SigmaPCBs from the Hudson River Estuary for the year of 2000.     

Fluxes of inorganic and organic arsenic species in a Norway spruce forest floor

To identify the role of the forest floor in arsenic (As) biogeochemistry, concentrations and fluxes of inorganic and organic As in throughfall, litterfall and forest floor percolates at different layers were investigated. Nearly 40% of total As(total) input (5.3g Asha(-1)yr(-1)) was retained in Oi layer, whereas As(total) fluxes from Oe and Oa layers exceeded the input by far (10.8 and 20g Asha(-1)yr(-1), respectively). Except dimethylarsinic acid (DMA), fluxes of organic As decreased with depth of forest floor so that <10% of total deposition (all <0.3g Asha(-1)yr(-1)) reached the mineral soil. All forest floor layers are sinks for most organic As. Conversely, Oe and Oa layers are sources of As(total), arsenite, arsenate and DMA. Significant correlations (r>/=0.43) between fluxes of As(total), arsenite, arsenate or DMA and water indicate hydrological conditions and adsorption-desorption as factors influencing their release from the forest floor. The higher net release of arsenite from Oe and Oa and of DMA from Oa layer in the growing than dormant season also suggests microbial influences on the release of arsenite and DMA.     

Particle fluxes above forests: observations, methodological considerations and method comparisons

This paper reports a study designed to test, evaluate and compare micro-meteorological methods for determining the particle number flux above forest canopies. Half-hour average particle number fluxes above a representative broad-leaved forest in Denmark derived using eddy covariance range from -7x10(7) m(-2) s(-1) (1st percentile) to 5x10(7) m(-2) s(-1) (99th percentile), and have a median value of -1.6x10(6) m(-2) s(-1). The statistical uncertainties associated with the particle number flux estimates are larger than those for momentum fluxes and imply that in this data set approximately half of the particle number fluxes are not statistically different to zero. Particle number fluxes from relaxed eddy accumulation (REA) and eddy covariance are highly correlated and of almost identical magnitude. Flux estimates from the co-spectral and dissipation methods are also correlated with those from eddy covariance but exhibit higher absolute magnitude of fluxes.     

Air-surface exchange of mercury with soils amended with ash materials

Air-surface exchange of mercury (Hg) was measured from soil low in Hg (0.013 mg/kg) amended with four different ash materials: a wood ash containing -10% coal ash (0.070 mg/kg Hg), a mixture of two subbituminous coal fly ashes (0.075 mg/kg Hg), a subbituminous coal ash containing -10% petroleum coke ash (1.2 mg/kg Hg), and an ash from incinerated municipal sewage sludge (4.3 mg/kg Hg) using a dynamic flux chamber. Ash was added to soil to simulate agricultural supplements, soil stabilization, and pad layers used in livestock areas. For the agricultural amendment, -0.4% ash was well mixed into the soil. To make the stabilized soil that could be used for construction purposes, -20% ash was mixed into soil with water. The pad layer consisted of a wetted 1-cm layer of ash material on the soil surface. Diel trends of Hg flux were observed for all of the substrates with significantly higher Hg emissions during the day and negligible flux or deposition of Hg during the night. Hg fluxes, which were measured in the summer months, were best correlated with solar radiation, temperature, and air O3 concentrations. Mean Hg fluxes measured outdoors for unamended soils ranged from 19 to 140 ng/m2 day, whereas those for soil amended with ash to simulate an agricultural application ranged from 7.2 to 230 ng/m2 day. Fluxes for soil stabilized with ash ranged from 77 to 530 ng/m2 day and for soil with pads constructed of ash ranged from -50 to 90 ng/m2 day. Simple analytical tests (i.e., total Hg content, synthetic precipitation leaching procedure, heating, and indoor gas-exchange experiments) were performed to assess whether algorithms based on these tests could be used to predict Hg fluxes observed outdoors using the flux chamber. Based on this study, no consistent relationships could be developed. More work is needed to assess long-term and seasonal variations in Hg flux from (intact and disturbed) substrates before annual estimates of emissions can be developed.