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Permafrost degradation is delivering bioavailable dissolved organic matter (DOM) and inorganic nutrients to surface water networks. While these permafrost subsidies represent a small portion of total fluvial DOM and nutrient fluxes, they could influence food webs and net ecosystem carbon balance via priming or nutrient effects that destabilize background DOM. We investigated how addition of biolabile carbon (acetate) and inorganic nutrients (nitrogen and phosphorus) affected DOM decomposition with 28‐day incubations. We incubated late‐summer stream water from 23 locations nested in seven northern or high‐altitude regions in Asia, Europe, and North America. DOM loss ranged from 3% to 52%, showing a variety of longitudinal patterns within stream networks. DOM optical properties varied widely, but DOM showed compositional similarity based on Fourier transform ion cyclotron resonance mass spectrometry (FT‐ICR MS) analysis. Addition of acetate and nutrients decreased bulk DOM mineralization (i.e., negative priming), with more negative effects on biodegradable DOM but neutral or positive effects on stable DOM. Unexpectedly, acetate and nutrients triggered breakdown of colored DOM (CDOM), with median decreases of 1.6% in the control and 22% in the amended treatment. Additionally, the uptake of added acetate was strongly limited by nutrient availability across sites. These findings suggest that biolabile DOM and nutrients released from degrading permafrost may decrease background DOM mineralization but alter stoichiometry and light conditions in receiving waterbodies. We conclude that priming and nutrient effects are coupled in northern aquatic ecosystems and that quantifying two‐way interactions between DOM properties and environmental conditions could resolve conflicting observations about the drivers of DOM in permafrost zone waterways., Key Points Dissolved organic matter (DOM) from diverse circumpolar regions showed compositional and optical commonalitiesAdded acetate and nutrients suppressed background DOM degradation but accelerated colored DOM breakdownDisconnect between DOM composition and function indicates intrinsic and extrinsic conditions interact to regulate DOM dynamics

Riverine ecosystems receive organic matter (OM) from terrestrial sources, internally produce new OM, and biogeochemically cycle and modify organic and inorganic carbon. Major gaps remain in the understanding of the relationships between carbon sources and processing in river systems. Here we synthesize isotopic, elemental, and molecular properties of dissolved organic carbon (DOC), particulate organic carbon (POC), and dissolved inorganic carbon (DIC) in the Upper Mississippi River (UMR) system above Wabasha, MN, including the main stem Mississippi River and its four major tributaries (Minnesota, upper Mississippi, St. Croix, and Chippewa Rivers). Our goal was to elucidate how biological processing modifies the chemical and isotopic composition of aquatic carbon pools during transport downstream in a large river system with natural and man-made impoundments. Relationships between land cover and DOC carbon-isotope composition, absorbance, and hydrophobic acid content indicate that DOC retains terrestrial carbon source information, while the terrestrial POC signal is largely replaced by autochthonous organic matter, and DIC integrates the influence of in-stream photosynthesis and respiration of organic matter. The UMR is slightly heterotrophic throughout the year, but pools formed by low-head navigation dams and natural impoundments promote a shift towards autotrophic conditions, altering aquatic ecosystem dynamics and POC and DIC composition. Such changes likely occur in all major river systems affected by low-head dams and need to be incorporated into our understanding of inland water carbon dynamics and processes controlling CO2 emissions from rivers, as new navigation and flood control systems are planned for future river and water resources management.

Boreal soils in permafrost regions contain vast quantities of frozen organic material that is released to terrestrial and aquatic environments via subsurface flow paths as permafrost thaws. Longer flow paths may allow chemical reduction of solutes, nutrients, and contaminants, with implications for greenhouse gas emissions and aqueous export. Predicting boreal catchment runoff is complicated by soil heterogeneities related to variability in active layer thickness, soil type, fire history, and preferential flow potential. By coupling measurements of permeability, infiltration potential, and water chemistry with a stream chemistry end-member mixing model, we tested the hypothesis that organic soils and burned slopes are the primary sources of runoff, and that runoff from burned soils is greater due to increased hydraulic connectivity. Organic soils were more permeable than mineral soils, and 25% of infiltration moved laterally upon reaching the organic-mineral soil boundary on unburned hillslopes. A large portion of the remaining water infiltrated into deeper, less permeable soils. In contrast, burned hillslopes displayed poorly defined soil horizons, allowing rapid, mineral-rich runoff through preferential pathways at various depths. On the catchment scale, mineral/organic runoff ratios averaged 1.6 and were as high as 5.2 for an individual storm. Our results suggest that burned soils are the dominant source of water and solutes reaching the stream in summer, whereas unburned soils may provide longer term storage and residence times necessary for production of anaerobic compounds. These results are relevant to predicting how boreal catchment drainage networks and stream export will evolve given continued warming and altered fire regimes.

Wetlands are the largest natural source of atmospheric methane. Here, we assess controls on methane flux using a database of approximately 19 000 instantaneous measurements from 71 wetland sites located across subtropical, temperate, and northern high latitude regions. Our analyses confirm general controls on wetland methane emissions from soil temperature, water table, and vegetation, but also show that these relationships are modified depending on wetland type (bog, fen, or swamp), region (subarctic to temperate), and disturbance. Fen methane flux was more sensitive to vegetation and less sensitive to temperature than bog or swamp fluxes. The optimal water table for methane flux was consistently below the peat surface in bogs, close to the peat surface in poor fens, and above the peat surface in rich fens. However, the largest flux in bogs occurred when dry 30-day averaged antecedent conditions were followed by wet conditions, while in fens and swamps, the largest flux occurred when both 30-day averaged antecedent and current conditions were wet. Drained wetlands exhibited distinct characteristics, e.g. the absence of large flux following wet and warm conditions, suggesting that the same functional relationships between methane flux and environmental conditions cannot be used across pristine and disturbed wetlands. Together, our results suggest that water table and temperature are dominant controls on methane flux in pristine bogs and swamps, while other processes, such as vascular transport in pristine fens, have the potential to partially override the effect of these controls in other wetland types. Because wetland types vary in methane emissions and have distinct controls, these ecosystems need to be considered separately to yield reliable estimates of global wetland methane release.

[1] Boreal ecosystems store significant quantities of organic carbon (C) that may be vulnerable to degradation as a result of a warming climate. Despite their limited coverage on the landscape, streams play a significant role in the processing, gaseous emission, and downstream export of C, and small streams are thought to be particularly important because of their close connection with the surrounding landscape. However, ecosystem carbon studies do not commonly incorporate the role of the aquatic conduit. We measured carbon dioxide (CO2) and methane (CH4) concentrations and emissions in a headwater stream network of interior Alaska underlain by permafrost to assess the potential role of stream gas emissions in the regional carbon balance. First-order streams exhibited the greatest variability in fluxes of CO2 and CH4, and the greatest mean pCO2. High-resolution time series of stream pCO2 and discharge at two locations on one first-order stream showed opposing pCO2 responses to storm events, indicating the importance of hydrologic flowpaths connecting CO2-rich soils with surface waters. Repeated longitudinal surveys on the stream showed consistent areas of elevated pCO2 and pCH4, indicative of discrete hydrologic flowpaths delivering soil water and groundwater having varying chemistry. Up-scaled basin estimates of stream gas emissions suggest that streams may contribute significantly to catchment-wide CH4 emissions. Overall, our results indicate that while stream-specific gas emission rates are disproportionately high relative to the terrestrial landscape, both stream surface area and catchment normalized emission rates were lower than those documented for the Yukon River Basin as a whole. This may be due to limitations of C sources and/or C transport to surface waters.

Carbon dynamics of high-latitude regions are an important and highly uncertain component of global carbon budgets, and efforts to constrain estimates of soil-atmosphere carbon exchange in these regions are contingent on accurate representations of spatial and temporal variability in carbon fluxes. This study explores spatial and temporal variability in soilatmosphere carbon dynamics at both fine and coarse spatial scales in a high-elevation, permafrost-dominated boreal black spruce forest. We evaluate the importance of landscape-level investigations of soil-atmosphere carbon dynamics by characterizing seasonal trends in soil-atmosphere carbon exchange, describing soil temperature-moisture-respiration relations, and quantifying temporal and spatial variability at two spatial scales: the plot scale (0–5 m) and the landscape scale (500–1000 m). Plot-scale spatial variability (average variation on a given measurement day) in soil CO2 efflux ranged from a coefficient of variation (CV) of 0.25 to 0.69,...

Recent warming at high-latitudes has accelerated permafrost thaw in northern peatlands, and thaw can have profound effects on local hydrology and ecosystem carbon balance. To assess the impact of permafrost thaw on soil organic carbon (OC) dynamics, we measured soil hydrologic and thermal dynamics and soil OC stocks across a collapse-scar bog chronosequence in interior Alaska. We observed dramatic changes in the distribution of soil water associated with thawing of ice-rich frozen peat. The impoundment of warm water in collapse-scar bogs initiated talik formation and the lateral expansion of bogs over time. On average, Permafrost Plateaus stored 137 ± 37 kg C m -2 , whereas OC storage in Young Bogs and Old Bogs averaged 84 ± 13 kg C m -2 . Based on our reconstructions, the accumulation of OC in near-surface bog peat continued for nearly 1,000 years following permafrost thaw, at which point accumulation rates slowed. Rapid decomposition of thawed forest peat reduced deep OC stocks by nearly half during the first 100 years following thaw. Using a simple mass-balance model, we show that accumulation rates at the bog surface were not sufficient to balance deep OC losses, resulting in a net loss of OC from the entire peat column. An uncertainty analysis also revealed that the magnitude and timing of soil OC loss from thawed forest peat depends substantially on variation in OC input rates to bog peat and variation in decay constants for shallow and deep OC stocks. These findings suggest that permafrost thaw and the subsequent release of OC from thawed peat will likely reduce the strength of northern permafrost-affected peatlands as a carbon dioxide sink, and consequently, will likely accelerate rates of atmospheric warming.

Black spruce forests are a dominant covertype in the boreal forest region, and they inhabit landscapes that span a wide range of hydrologic and thermal conditions. These forests often have large stores of soil organic carbon. Recent increases in temperature at northern latitudes may be stimulating decomposition rates of this soil carbon. It is unclear, however, how changes in environmental conditions influence decomposition in these systems, and if substrate controls of decomposition vary with hydrologic and thermal regime. We addressed these issues by investigating the effects of temperature, moisture, and organic matter chemical characteristics on decomposition of fibric soil horizons from three black spruce forest sites. The sites varied in drainage and permafrost, and included a “Well Drained” site where permafrost was absent, and “Moderately well Drained” and “Poorly Drained” sites where permafrost was present at about 0.5 m depth. Samples collected from each site were incubated at five different moisture contents (2, 25, 50, 75, and 100% saturation) and two different temperatures (10°C and 20°C) in a full factorial design for two months. Organic matter chemistry was analyzed using pyrolysis gas chromatography-mass spectrometry prior to incubation, and after incubation on soils held at 20°C, 50% saturation. Mean cumulative mineralization, normalized to initial carbon content, ranged from 0.2% to 4.7%, and was dependent on temperature, moisture, and site. The effect of temperature on mineralization was significantly influenced by moisture content, as mineralization was greatest at 20°C and 50–75% saturation. While the relative effects of temperature and moisture were similar for all soils, mineralization rates were significantly greater for samples from the “Well Drained” site compared to the other sites. Variations in the relative abundances of polysaccharide-derivatives and compounds of undetermined source (such as toluene, phenol, 4-methyl phenol, and several unidentifiable compounds) could account for approximately 44% of the variation in mineralization across all sites under ideal temperature and moisture conditions. Based on our results, changes in temperature and moisture likely have similar, additive effects on in situ soil organic matter (SOM) decomposition across a wide range of black spruce forest systems, while variations in SOM chemistry can lead to significant differences in decomposition rates within and among forest sites.

Mercury (Hg) emission and deposition can occur to and from soils, and are an important component of the global atmospheric Hg budget. This paper focuses on synthesizing existing surface-air Hg flux data collected throughout the Western North American region and is part of a series of geographically focused Hg synthesis projects. A database of existing Hg flux data collected using the dynamic flux chamber (DFC) approach from almost a thousand locations was created for the Western North America region. Statistical analysis was performed on the data to identify the important variables controlling Hg fluxes and to allow spatiotemporal scaling. The results indicated that most of the variability in soil-air Hg fluxes could be explained by variations in soil-Hg concentrations, solar radiation, and soil moisture. This analysis also identified that variations in DFC methodological approaches were detectable among the field studies, with the chamber material and sampling flushing flow rate influencing the magnitude of calculated emissions. The spatiotemporal scaling of soil-air Hg fluxes identified that the largest emissions occurred from irrigated agricultural landscapes in California. Vegetation was shown to have a large impact on surface-air Hg fluxes due to both a reduction in solar radiation reaching the soil as well as from direct uptake of Hg in foliage. Despite high soil Hg emissions from some forested and other heavily vegetated regions, the net ecosystem flux (soil flux + vegetation uptake) was low. Conversely, sparsely vegetated regions showed larger net ecosystem emissions, which were similar in magnitude to atmospheric Hg deposition (except for the Mediterranean California region where soil emissions were higher). The net ecosystem flux results highlight the important role of landscape characteristics in effecting the balance between Hg sequestration and (re-)emission to the atmosphere.

Carbon dioxide (CO2) accumulates under lake ice in winter and degasses to the atmosphere after ice melt. This large springtime CO2 pulse is not typically considered in surface-atmosphere flux estimates, because most field studies have not sampled through ice during late winter. Measured CO2 partial pressure (pCO2) of lake surface water ranged from 8.6 to 4,290 Pa (85–4,230 µatm) in 234 north temperate and boreal lakes prior to ice melt during 1998 and 1999. Only four lakes had surface pCO2 less than or equal to atmospheric pCO2, whereas 75% had pCO2 >5 times atmospheric. The δ13CDIC (DIC = ΣCO2) of 142 of the lakes ranged from –26.28‰ to +0.95‰. Lakes with the greatest pCO2 also had the lightest δ13CDIC, which indicates respiration as their primary CO2 source. Finnish lakes that received large amounts of dissolved organic carbon from surrounding peatlands had the greatest pCO2. Lakes set in noncarbonate till and bedrock in Minnesota and Wisconsin had the smallest pCO2 and the heaviest d13CDIC, which indicates atmospheric and/or mineral sources of C for those lakes. Potential emissions for the period after ice melt were 2.36 ± 1.44 mol CO2 m−2 for lakes with average pCO2 values and were as large as 13.7 ± 8.4 mol CO2 m−2 for lakes with high pCO2 values.

Carbon dioxide (CO2) and methane (CH4) exchange between the atmosphere and a subalpine wetland located in Rocky Mountain National Park, Colorado, at 3200 m elevation were measured during 1996–1998. Respiration, net CO2 flux, and CH4 flux were measured using the closed chamber method during snow-free periods and using gas diffusion calculations during snow-covered periods. The ranges of measured flux were 1.2-526 mmol CO2 m−2 d−1 (respiration), −1056−100 mmol CO2m−2 d−1 (net CO2exchange), and 0.1–36.8 mmol CH4m−2 d−1 (a positive value represents efflux to the atmosphere). Respiration and CH4 emission were significantly correlated with 5 cm soil temperature. Annual respiration and CH4 emission were modeled by applying the flux-temperature relationships to a continuous soil temperature record during 1996–1998. Gross photosynthesis was modeled using a hyperbolic equation relating gross photosynthesis, photon flux density, and soil temperature. Modeled annual flux estimates indicate that the wetland was a net source of carbon gas to the atmosphere each of the three years: 8.9 mol C m−2 yr−1 in 1996, 9.5 mol C m−2 yr−1 in 1997, and 9.6 mol C m−2 yr−1 in 1998. This contrasts with the long-term carbon accumulation of ∼0.7 mol m−2 yr−1 determined from 14C analyses of a peat core collected from the wetland.

Methane exchange between the atmosphere and subalpine wetland and unsaturated soils was evaluated over a 15-month period during 1995-1996. Four vegetation community types along a moisture gradient (wetland, moist-grassy, moist-mossy, and dry) were included in a 100 m sampling transect situated at 3200 m elevation in Rocky Mountain National Park, Colorado. Methane fluxes and soil temperature were measured during snow-free and snow-covered periods, and soil moisture content was measured during snow-free periods. The range of mean measured fluxes through all seasons (a positive value represents CH 4 efflux to the atmosphere) were: 0.3 to 29.2 mmol CH 4 m -2 d -1 wetland area; 0. 1 to 1.8 mmol CH 4 m -2 d -1 , moist-grassy area; -0.04 to 0.7 mmol CH 4 m -2 d -1 , moist-mossy area; and -0.6 to 0 mmol CH 4 m -2 d -1 , dry area. Methane efflux was significantly correlated with soil temperature (5 cm) at the continuously saturated wetland area during snow-free periods. Consumption of atmospheric methane was significantly correlated with moisture content in the upper 5 cm of soil at the dry area. A model based on the wetland flux-temperature relationship estimated an annual methane emission of 2.53 mo CH 4 m -2 from the wetland. Estimates of annual methane flux based on field measurements at the other sites were 0.12 mol CH 4 m -2 , moist-grassy area; 0.03 mol CH 4 m -2 , moist-mossy area; and -0.04 mol CH 4 m -2 , dry area. Methane fluxes during snow-covered periods were responsible for 25, 73, 23, and 43% of the annual fluxes at the wetland, moist-grassy, moist-mossy, and dry sites, respectively.

Fluxes of CO2 and CH 4 through a seasonal snowpack were measured in and adjacent to a subalpine wetland in Rocky Mountain National Park, Colorado. Gas diffusion through the snow was controlled by gas production or consumption in the soil and by physical snowpack properties. The snowpack insulated soils from cold midwinter air temperatures allowing microbial activity to continue through the winter. All soil types studied were net sources of CO2 to the atmosphere through the winter, whereas saturated soils in the wetland center were net emitters of CH 4 and soils adjacent to the wetland were net CH 4 consumers. Most sites showed similar temporal patterns in winter gas fluxes; the lowest fluxes occurred in early winter, and maximum fluxes occurred at the onset of snowmelt. Temporal changes in fluxes probably were related to changes in soil-moisture conditions and hydrology because soil temperatures were relatively constant under the snowpack. Average winter CO2 fluxes were 42.3, 31.2, and 14.6 mmol m -2 d -• over dry, moist, and saturated soils, respectively, which accounted for 8 to 23% of the gross annual CO2 emissions from these soils. Average winter CH 4 fluxes were -0.016, 0.274, and 2.87 mmol m -2 d -1 over dry, moist, and saturated soils, respectively. Microbial activity under snow cover accounted for 12% of the annual CH 4 consumption in dry soils and 58 and 12% of the annual CH 4 emitted from moist and saturated soils, respectively. The observed ranges in CO2 and CH 4 flux through snow indicated that winter fluxes are an important part of the annual carbon budget in seasonally snow-covered terrains.

[1] Northern high-latitude rivers transport large amounts of terrestrially derived dissolved organic matter (DOM) from boreal and arctic ecosystems to coastal areas and oceans. Current knowledge of the biodegradability of DOM in these rivers is limited, particularly for large rivers discharging to the Arctic Ocean. We conducted a seasonally comprehensive study of biodegradable dissolved organic carbon (BDOC) dynamics in the Yukon River and two of its tributaries in Alaska, USA. Distinct seasonal patterns of BDOC, consistent across a wide range of watershed size, indicate BDOC is transported year-round. Relative biodegradability (%BDOC) was greatest during winter, and decreased into spring and summer. Due to large seasonal differences in DOC concentration, the greatest concentrations of BDOC (mg C L−1) occurred during spring freshet, followed by winter and summer. While chemical composition of DOM was an important driver of BDOC, the overriding control of BDOC was mineral nutrient availability due to wide shifts in carbon (C) and nitrogen (N) stoichiometry across seasons. We calculated seasonal and annual loads of BDOC exported by the Yukon River by applying measured BDOC concentrations to daily water discharge values, and also by applying an empirical correlation between %BDOC and the ratio of DOC to dissolved inorganic N (DIN) to total DOC loads. The Yukon River exports ∼0.2 Tg C yr−1 as BDOC that is decomposable within 28 days. This corresponds to 12–18% of the total annual DOC export. Furthermore, we calculate that the six largest arctic rivers, including the Yukon River, collectively export ∼2.3 Tg C yr−1 as BDOC to the Arctic Ocean.

[1] The seasonal and spatial variability of dissolved organic matter (DOM) quantity and chemical composition were investigated in the Yukon River basin of Alaska, United States, and northwestern Canada. Dissolved organic carbon (DOC), chromophoric DOM (CDOM), and dissolved lignin phenols were measured across a range of source waters and the seasonal hydrograph. Strong relationships were determined between CDOM and both DOC and lignin phenols, highlighting the potential for deriving detailed spatial and temporal distributions of DOM composition from CDOM monitoring. Maximum concentrations of measured parameters were observed during the spring flush, when DOM had a remarkably high content of aromatic vascular plant material derived from surface soil and litter layers. A larger portion of riverine DOM was attributed to vascular plant sources than previously believed by utilizing representative vegetation leachates and a soil pore water as end-members. In combination with recent studies highlighting export of young, labile DOM during the spring flush in northern high-latitude river systems, our results suggest riverine DOM is less degraded and more labile than previously thought with clear ramifications for its biomineralization or photo-oxidation in marine environments.

[1] Loads and yields of dissolved and particulate organic and inorganic carbon (DOC, POC, DIC, PIC) were measured and modeled at three locations on the Yukon River (YR) and on the Tanana and Porcupine rivers (TR, PR) in Alaska during 2001–2005. Total YR carbon export averaged 7.8 Tg C yr−1, 30% as OC and 70% as IC. Total C yields (0.39–1.03 mol C m−2 yr−1) were proportional to water yields (139–356 mm yr−1; r2 = 0.84) at all locations. Summer DOC had an aged component (fraction modern (FM) = 0.94–0.97), except in the permafrost wetland-dominated PR, where DOC was modern. POC had FM = 0.63–0.70. DOC had high concentration, high aromaticity, and high hydrophobic content in spring and low concentration, low aromaticity, and high hydrophilic content in winter. About half of annual DOC export occurred during spring. DIC concentration and isotopic composition were strongly affected by dissolution of suspended carbonates in glacial meltwater during summer.

[1] Permafrost melting is occurring in areas of the boreal forest region where large amounts of carbon (C) are stored in organic soils. We measured soil respiration, net CO2 flux, and net CH4 flux during May–September 2003 and March 2004 in a black spruce lowland in interior Alaska to better understand how permafrost thaw in poorly drained landscapes affects land-atmosphere CO2 and CH4 exchange. Sites included peat soils underlain by permafrost at ∼0.4 m depth (permafrost plateau, PP), four thermokarst wetlands (TW) having no permafrost in the upper 2.2 m, and peat soils bordering the thermokarst wetlands having permafrost at ∼0.5 m depth (thermokarst edges, TE). Soil respiration rates were not significantly different among the sites, and 5-cm soil temperature explained 50–91% of the seasonal variability in soil respiration within the sites. Groundcover vegetation photosynthesis (calculated as net CO2 minus soil respiration) was significantly different among the sites (TW > TE > PP), which can be partly attributed to the difference in photosynthetically active radiation reaching the ground at each site type. Methane emission rates were 15 to 28 times greater from TW than from TE and PP. We modeled annual soil respiration and groundcover vegetation photosynthesis using soil temperature and radiation data, and CH4 flux by linear interpolation. We estimated all sites as net C gas sources to the atmosphere (not including tree CO2 uptake at PP and TE), although the ranges in estimates when accounting for errors were large enough that TE and TW may have been net C sinks.