Heleen A. de Wit

Dissolved organic carbon trends resulting from changes in atmospheric deposition chemistry.

Several hypotheses have been proposed to explain recent, widespread increases in concentrations of dissolved organic carbon (DOC) in the surface waters of glaciated landscapes across eastern North America and northern and central Europe. Some invoke anthropogenic forcing through mechanisms related to climate change, nitrogen deposition or changes in land use, and by implication suggest that current concentrations and fluxes are without precedent. All of these hypotheses imply that DOC levels will continue to rise, with unpredictable consequences for the global carbon cycle. Alternatively, it has been proposed that DOC concentrations are returning toward pre-industrial levels as a result of a gradual decline in the sulphate content of atmospheric deposition. Here we show, through the assessment of time series data from 522 remote lakes and streams in North America and northern Europe, that rising trends in DOC between 1990 and 2004 can be concisely explained by a simple model based solely on changes in deposition chemistry and catchment acid-sensitivity. We demonstrate that DOC concentrations have increased in proportion to the rates at which atmospherically deposited anthropogenic sulphur and sea salt have declined. We conclude that acid deposition to these ecosystems has been partially buffered by changes in organic acidity and that the rise in DOC is integral to recovery from acidification. Over recent decades, deposition-driven increases in organic matter solubility may have increased the export of DOC to the oceans, a potentially important component of regional carbon balances. The increase in DOC concentrations in these regions appears unrelated to other climatic factors.

Testing seasonal and long-term controls of streamwater DOC using empirical and process-based models

Concentrations of dissolved organic carbon (DOC) in surface waters are increasing across Europe and parts of North America. Several mechanisms have been proposed to explain these increases including reductions in acid deposition, change in frequency of winter storms and changes in temperature and precipitation patterns. We used two modelling approaches to identify the mechanisms responsible for changing surface water DOC concentrations. Empirical regression analysis and INCA-C, a process-based model of stream-water DOC, were used to simulate long-term (1986--2003) patterns in stream water DOC concentrations in a small boreal stream. Both modelling approaches successfully simulated seasonal and inter-annual patterns in DOC concentration. In both models, seasonal patterns of DOC concentration were controlled by hydrology and inter-annual patterns were explained by climatic variation. There was a non-linear relationship between warmer summer temperatures and INCA-C predicted DOC. Only the empirical model was able to satisfactorily simulate the observed long-term increase in DOC. The observed long-term trends in DOC are likely to be driven by in-soil processes controlled by SO4(2-) and Cl(-) deposition, and to a lesser extent by temperature-controlled processes. Given the projected changes in climate and deposition, future modelling and experimental research should focus on the possible effects of soil temperature and moisture on organic carbon production, sorption and desorption rates, and chemical controls on organic matter solubility.

Mercury budget of a small forested boreal catchment in southeast Norway.

We present input and output fluxes of total mercury (Hg(tot)) and methyl mercury (MeHg) based on throughfall, litterfall and stream water samples from 2004/2005 from a small forested catchment (Langtjern) in Norway. Hg(tot) input via throughfall and litterfall was estimated to 6.7 and 2.7 microg m(-2) yr(-1), respectively, which is considerably lower than previously reported from other boreal catchments in Scandinavia. A likely cause for the low input flux is the sparseness and low productivity of the forest in the Langtjern catchment, with less atmospheric scavenging and lower litterfall fluxes than previously studied sites. In addition there has been a general decrease in mercury (Hg) in the atmosphere on the northern hemisphere in the last decade. The estimated output flux of Hg(tot) with surface water was 2.5 microg m(-2) yr(-1), which is comparable to what has been reported elsewhere. The ratio of Hg(tot) output flux to input flux was 26%, which is considerably higher than reported from other sites. This illustrates that catchment properties have greater importance for surface water export of Hg than the current atmospheric input. The estimated total soil pool of Hg(tot) in the catchment was 17.4 mg m(-2). This corresponds to roughly 8000 years of the current surface water output flux and 2000 years of the current input flux.

Climate warming feedback from mountain birch forest expansion: reduced albedo dominates carbon uptake

Expanding high-elevation and high-latitude forest has contrasting climate feedbacks through carbon sequestration (cooling) and reduced surface reflectance (warming), which are yet poorly quantified. Here, we present an empirically based projection of mountain birch forest expansion in south-central Norway under climate change and absence of land use. Climate effects of carbon sequestration and albedo change are compared using four emission metrics. Forest expansion was modeled for a projected 2.6 °C increase in summer temperature in 2100, with associated reduced snow cover. We find that the current (year 2000) forest line of the region is circa 100 m lower than its climatic potential due to land-use history. In the future scenarios, forest cover increased from 12% to 27% between 2000 and 2100, resulting in a 59% increase in biomass carbon storage and an albedo change from 0.46 to 0.30. Forest expansion in 2100 was behind its climatic potential, forest migration rates being the primary limiting factor. In 2100, the warming caused by lower albedo from expanding forest was 10 to 17 times stronger than the cooling effect from carbon sequestration for all emission metrics considered. Reduced snow cover further exacerbated the net warming feedback. The warming effect is considerably stronger than previously reported for boreal forest cover, because of the typically low biomass density in mountain forests and the large changes in albedo of snow-covered tundra areas. The positive climate feedback of high-latitude and high-elevation expanding forests with seasonal snow cover exceeds those of afforestation at lower elevation, and calls for further attention of both modelers and empiricists. The inclusion and upscaling of these climate feedbacks from mountain forests into global models is warranted to assess the potential global impacts.

From greening to browning: Catchment vegetation development and reduced S-deposition promote organic carbon load on decadal time scales in Nordic lakes

Increased concentrations of dissolved organic carbon (DOC), often labelled “browning”, is a current trend in northern, particularly boreal, freshwaters. The browning has been attributed to the recent reduction in sulphate (S) deposition during the last 2 to 3 decades. Over the last century, climate and land use change have also caused an increasing trend in vegetation cover (“greening”), and this terrestrially fixed carbon represents another potential source for export of organic carbon to lakes and rivers. The impact of this greening on the observed browning of lakes and rivers on decadal time scales remains poorly investigated, however. Here, we explore time-series both on water chemistry and catchment vegetation cover (using NDVI as proxy) from 70 Norwegian lakes and catchments over a 30-year period. We show that the increase in terrestrial vegetation as well as temperature and runoff significantly adds to the reduced SO4-deposition as a driver of freshwater DOC concentration. Over extended periods (centuries), climate mediated changes in vegetation cover may cause major browning of northern surface waters, with severe impact on ecosystem productivity and functioning.

Environmental factors influencing mercury speciation in Subarctic and Boreal lakes

Environmental drivers of total mercury (TotHg) concentrations, methylmercury (MeHg) concentrations, and MeHg fractions (a proxy for methylation potential, expressed as %MeHg) were assessed in a synoptic study of 51 lakes in southeast (Boreal) and northeast (Subarctic) Norway. Concentrations of TotHg and MeHg ranged between 0.5-6.6 ng/L and <0.02-0.70 ng/L, respectively. The lakes span wide ranges of explanatory environmental variables, including water chemistry, catchment characteristics, climate conditions, and atmospheric deposition of Hg, sulphur and nitrogen (N). Dissolved organic matter (DOM), measured as total organic carbon (TOC), was the variable most strongly correlated with TotHg (r(2)=0.76) and MeHg (r(2)=0.64) concentrations. Lakes in the Subarctic region had significantly lower TotHg and MeHg concentrations, and %MeHg than lakes in the Boreal region (p<0.01), implying a lower aquatic food web exposure of aqueous Hg species in Subarctic Norway than in the Boreal lakes. Statistical modelling (partial least squares) using data from the Boreal lakes produced models explaining 82%, 75% and 50% of the spatial variation of TotHg and MeHg concentrations and %MeHg, respectively. After TOC, the most significant explanatory variables were N availability, base cation status, and lake and catchment size. We conclude that a key process driving TotHg concentrations is DOM as a transport vector, while the role of DOM for MeHg and %MeHg is likely related to a combination of transport and DOM as a substrate for methylation. Also, negative correlations between MeHg, and catchment and lake size are consistent with in-lake and in-stream de-methylation processes. The statistical relationship suggests that N availability exerts a positive contribution on concentrations of MeHg and %MeHg.

Oxygen dynamics in a boreal lake responds to long-term changes in climate, ice phenology, and DOC inputs

Boreal lakes are impacted by climate change, reduced acid deposition, and changing loads of dissolved organic carbon (DOC) from catchments. We explored, using the process-based lake model MyLake, how changes in these pressures modulate ice phenology and the dissolved oxygen concentrations (DO) of a small boreal humic lake. The model was parametrized against year-round time series of water temperature and DO from a lake buoy. Observed trends in air temperature (+0.045°C yr−1) and DOC concentration (0.11 mg C L−1 yr−1, +1% annually) over the past 40 years were used as model forcings. A backcast of ice freezing and breakup dates revealed that ice breakup occurred on average 8 days earlier in 2014 than in 1974. The earlier ice breakup enhanced water column ventilation resulting in higher DO in the spring. Warmer water in late summer led to longer anoxic periods, as microbial DOC turnover increased. A long-term increase in DOC concentrations caused a decline in lake DO, leading to 15% more hypoxic days (<3 mg L−1) and 10% more anoxic days (<15 µg L−1) in 2014 than in 1974. We conclude that climate warming and increasing DOC loads are antagonistic with respect to their effect on DO availability. The model suggests that DOC is a stronger driver of DO consumption than temperature. The browning of lakes may thus cause reductions in the oxythermal habitat of fish and aquatic biota in boreal lakes.

Effects of sample preservation and storage on mercury speciation in natural stream water

Despite an increasing focus on low level methods for determination of mercury species in water over the last decades, few studies have paid attention to direct effects of different sample preparation methods (i.e. preservation techniques) on natural freshwater samples. In this study we show how different preservation techniques give significantly different concentrations of total and methylmercury in freshwaters (9 and 14% on average, respectively). Natural stream samples from a forested lake catchment were studied. Mean stream sample concentrations of total (3.6 ng/L) and methylmercury (0.06 ng/L) reflect levels typical for pristine humic boreal catchments. The main reason for the observed average differences in total and methylmercury concentrations is the use of one instead of two sample bottles and timing of sample acidification, respectively.

Methylmercury bioaccumulation in invertebrates of boreal streams in Norway: Effects of aqueous methylmercury and diet retention

Transfer of aqueous methylmercury (MeHg) to primary consumers in aquatic foodwebs is poorly understood despite its importance for bioaccumulation of MeHg. We studied bioaccumulation of MeHg in simple aquatic food chains of two humic boreal streams in relation to streamwater chemistry, food web characteristics and dietary fatty acid (FA) biomarkers. Transfer of aqueous MeHg into primary consumers was similar in both streams, resulting in higher MeHg in consumers in the MeHg-rich stream. Trophic enrichment of MeHg and dietary retention of FA biomarkers was the same in both streams, suggesting that exposure to aqueous MeHg at the base of the food chain determined levels of MeHg in biota. In addition, contents of dietary biomarkers suggested that ingestion of algae reduced MeHg bioaccumulation, while ingestion of bacteria stimulated MeHg uptake. Dietary uptake of bacteria could thus be an important pathway for MeHg-transfer at the bottom of food chains in humic streams.

Effect of Climate Change on Flux of N and C: Air-Land-Freshwater-Marine Links: Synthesis

Abstract Projected climate change might increase the deposition of nitrogen by about 10% to seminatural ecosystems in southern Norway. At Storgama, increased precipitation in the growing season increased the fluxes of total organic carbon (TOC) and total organic nitrogen (TON) in proportion to the water flux. In winter, soil temperatures near 0°C, common under a snowpack, induced higher runoff of inorganic nitrogen (N) and lower runoff of TOC. By contrast, soil temperatures below freezing, caused by little snow accumulation (expected in a warmer world), reduced runoff of inorganic N, TON, and TOC. Long-term monitoring data showed that reduced snowpack can cause either decreased or increased N leaching, depending on interactions with N deposition, soil temperature regime, and winter discharge. Seasonal variation in TOC was mainly climatically controlled, whereas deposition of sulfate and nitrate (NO3) explained the long-term TOC increase. Upscaling to the river basin scale showed that the annual flux of NO3 will remain unchanged in response to climate change projections.