Recent Submissions

  • Aquatic biomass is a major source to particulate organic matter export in large Arctic rivers

    Behnke, Megan; Tank, Suzanne; McClelland, James W.; Holmes, Robert M.; Haghipour, Negar; Eglinton, Timothy; Raymond, Peter A.; Suslova, Anya; Zhulidov, Alexander V.; Gurtovaya, Tatiana; et al. (National Academy of Sciences, 2023-03-13)
    Arctic rivers provide an integrated signature of the changing landscape and transmit signals of change to the ocean. Here, we use a decade of particulate organic matter (POM) compositional data to deconvolute multiple allochthonous and autochthonous pan-Arctic and watershed-specific sources. Constraints from carbon-to-nitrogen ratios (C:N), δ13C, and Δ14C signatures reveal a large, hitherto overlooked contribution from aquatic biomass. Separation in Δ14C age is enhanced by splitting soil sources into shallow and deep pools (mean ± SD: −228 ± 211 vs. −492 ± 173‰) rather than traditional active layer and permafrost pools (−300 ± 236 vs. −441 ± 215‰) that do not represent permafrost-free Arctic regions. We estimate that 39 to 60% (5 to 95% credible interval) of the annual pan-Arctic POM flux (averaging 4,391 Gg/y particulate organic carbon from 2012 to 2019) comes from aquatic biomass. The remainder is sourced from yedoma, deep soils, shallow soils, petrogenic inputs, and fresh terrestrial production. Climate change-induced warming and increasing CO2 concentrations may enhance both soil destabilization and Arctic river aquatic biomass production, increasing fluxes of POM to the ocean. Younger, autochthonous, and older soil-derived POM likely have different destinies (preferential microbial uptake and processing vs. significant sediment burial, respectively). A small (~7%) increase in aquatic biomass POM flux with warming would be equivalent to a ~30% increase in deep soil POM flux. There is a clear need to better quantify how the balance of endmember fluxes may shift with different ramifications for different endmembers and how this will impact the Arctic system.
  • The role of glacier erosion in riverine particulate organic carbon export

    Behnke, Megan; Fellman, Jason B.; Nagorski, Sonia; Spencer, Robert G. M.; Hood, Eran (American Geophysical Union, 2023-11-01)
    Biospheric particulate organic carbon (POCbio) burial and rock petrogenic particulate organic carbon (POCpetro) oxidation are opposing long-term controls on the global carbon cycle, sequestering and releasing carbon, respectively. Here, we examine how watershed glacierization impacts the POC source by assessing the concentration and isotopic composition (δ13C and Δ14C) of POC exported from four watersheds with 0%–49% glacier coverage across a melt season in Southeast Alaska. We used two mixing models (age-weight percent and dual carbon isotope) to calculate concentrations of POCbio and POCpetro within the bulk POC pool. The fraction POCpetro contribution was highest in the heavily glacierized watershed (age-weight percent: 0.39 ± 0.05; dual isotope: 0.42 (0.37–0.47)), demonstrating a glacial source of POCpetro to fjords. POCpetro was mobilized via glacier melt and subglacial flow, while POCbio was largely flushed from the non-glacierized landscape by rain. Flow normalized POCbio concentrations exceeded POCpetro concentrations for all streams, but surprisingly were highest in the heavily glacierized watershed (mean: 0.70 mgL−1; range 0.16–1.41 mgL−1), suggesting that glacier rivers can contribute substantial POCbio to coastal waters. Further, the most heavily glacierized watershed had the highest sediment concentration (207 mgL−1; 7–708 mgL−1), and thus may facilitate long-term POCbio protection via sediment burial in glacier-dominated fjords. Our results suggest that continuing glacial retreat will decrease POC concentrations and increase POCbio:POCpetro exported from currently glacierized watersheds. Glacier retreat may thus decrease carbon storage in marine sediments and provide a positive feedback mechanism to climate change that is sensitive to future changes in POCpetro oxidation.
  • Trees in the stream: Determining patterns of terrestrial dissolved organic matter contributions to the Northeast Pacific Coastal Temperate Rainforest

    Behnke, Megan; Fellman, Jason B.; D'Amore, David V.; Spencer, Robert G. M. (American Geophysical Union, 2023-04-10)
    Dissolved organic matter (DOM) composition in small watersheds depends on complex antecedent conditions that ultimately influence DOM generation, processing, and stability downstream. Here, we used ultrahigh resolution Fourier-transform ion cyclotron resonance mass spectrometry and total dissolved nitrogen and dissolved organic carbon concentrations to investigate how DOM is produced in distinct sub-catchment types (poor fen, forested wetland, and upland forest) and transported through a watershed in the northeast Pacific coastal temperate rainforest (NPCTR). We traced a suite of previously identified source-specific marker formulae from vegetation and soil downstream and used them to test models of terrestrial DOM inputs. Marker formulae escaped microbial degradation and were exported from the watershed, demonstrating strong land-to-ocean connectivity through the transfer of unmodified tree DOM from specific tree species into the marine environment. Simple hydrologic and temperature variables were better able to predict inputs of soil-sourced DOM into the stream network than tree-sourced DOM, highlighting the role of antecedent conditions (e.g., plant growth stage) in DOM source availability and hydrologic flow connectivity, particularly for plant-derived material. Forested wetland pore waters featured thousands of nitrogen-containing molecular formulae that potentially provide a path of direct organic nitrogen uptake to organisms. The modified aromaticity index peaked in midsummer (up to 0.55 for fen headwaters) suggesting DOM inputs from freshly produced vegetation provide a strong summertime terrestrial signal. As the climate changes, new watershed-scale conditions may further complicate predictions of DOM source availability, flow connectivity, and downstream fate in NPCTR watersheds.
  • A new conceptual framework for the transformation of groundwater dissolved organic matter

    McDonough, Liza K.; Andersen, Martin S.; Behnke, Megan; Rutlidge, Helen; Oudone, Phetdala; Meredith, Karina; O’Carrol, Denis M.; Santos, Isaac R.; Marjo, Christopher E.; Spencer, Robert G. M.; et al. (Nature Communications, 2022-04-20)
    Groundwater comprises 95% of the liquid fresh water on Earth and contains a diverse mix of dissolved organic matter (DOM) molecules which play a significant role in the global carbon cycle. Currently, the storage times and degradation pathways of groundwater DOM are unclear, preventing an accurate estimate of groundwater carbon sources and sinks for global carbon budgets. Here we reveal the transformations of DOM in aging groundwater using ultra-high resolution mass spectrometry combined with radiocarbon dating. Long-term anoxia and a lack of photodegradation leads to the removal of oxidised DOM and a build-up of both reduced photodegradable formulae and aerobically biolabile formulae with a strong microbial signal. This contrasts with the degradation pathway of DOM in oxic marine, river, and lake systems. Our findings suggest that processes such as groundwater extraction and subterranean groundwater discharge to oceans could result in up to 13 Tg of highly photolabile and aerobically biolabile groundwater dissolved organic carbon released to surface environments per year, where it can be rapidly degraded. These findings highlight the importance of considering groundwater DOM in global carbon budgets.
  • From canopy to consumer: what makes and modifes terrestrial DOM in a temperate forest

    Behnke, Megan; Fellman, Jason B.; D'Amore, David V.; Gomez, S. M.; Spencer, R. G. M. (Springer, 2022-03-02)
    To investigate how source and processing control the composition of “terrestrial” dissolved organic matter (DOM), we combine soil and tree leachates, tree DOM, laboratory bioincubations, and ultrahigh resolution Fourier-transform ion cyclotron resonance mass spectrometry in three common landscape types (upland forest, forested wetland, and poor fen) of Southeast Alaska’s temperate rainforest. Tree (Tsuga heterophylla and Picea sitchensis) needles and bark and soil layers from each site were leached, and tree stemflow and throughfall collected to examine DOM sources. Dissolved organic carbon concentrations were as high as 167 mg CL−1 for tree DOM, suggesting tree DOM fluxes may be substantial given the hypermaritime climate of the region. Condensed aromatics contributed as much as 38% relative abundance of spruce and hemlock bark leachates suggesting coniferous trees are potential sources of condensed aromatics to surface waters. Soil leachates showed soil wetness dictates DOM composition and processing, with wetland soils producing more aromatic formulae and allowing the preservation of traditionally biolabile, aliphatic formulae. Biodegradation impacted soil and tree DOM differently, and though the majority of source-specific marker formulae were consumed for all sources, some marker formulae persisted. Tree DOM was highly biolabile (> 50%) and showed compositional convergence where processing homogenized DOM from different tree sources. In contrast, wetland and upland soil leachate DOM composition diverged and processing diversified DOM from different soil sources during bioincubations. Increasing precipitation intensity predicted with climate change in Southeast Alaska will increase tree leaching and soil DOM flushing, tightening linkages between terrestrial sources and DOM export to the coastal ocean.
  • From canopy to consumer: what makes and modifies terrestrial DOM in a temperate forest

    Behnke, Megan; Fellman, Jason B.; D'Amore, David V.; Gomez, S. M.; Spencer, R. G. M. (Springer, 2022-03-02)
    To investigate how source and processing control the composition of “terrestrial” dissolved organic matter (DOM), we combine soil and tree leachates, tree DOM, laboratory bioincubations, and ultrahigh resolution Fourier-transform ion cyclotron resonance mass spectrometry in three common landscape types (upland forest, forested wetland, and poor fen) of Southeast Alaska’s temperate rainforest. Tree (Tsuga heterophylla and Picea sitchensis) needles and bark and soil layers from each site were leached, and tree stemflow and throughfall collected to examine DOM sources. Dissolved organic carbon concentrations were as high as 167 mg CL−1 for tree DOM, suggesting tree DOM fluxes may be substantial given the hypermaritime climate of the region. Condensed aromatics contributed as much as 38% relative abundance of spruce and hemlock bark leachates suggesting coniferous trees are potential sources of condensed aromatics to surface waters. Soil leachates showed soil wetness dictates DOM composition and processing, with wetland soils producing more aromatic formulae and allowing the preservation of traditionally biolabile, aliphatic formulae. Biodegradation impacted soil and tree DOM differently, and though the majority of source-specific marker formulae were consumed for all sources, some marker formulae persisted. Tree DOM was highly biolabile (> 50%) and showed compositional convergence where processing homogenized DOM from different tree sources. In contrast, wetland and upland soil leachate DOM composition diverged and processing diversified DOM from different soil sources during bioincubations. Increasing precipitation intensity predicted with climate change in Southeast Alaska will increase tree leaching and soil DOM flushing, tightening linkages between terrestrial sources and DOM export to the coastal ocean.