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  • Biomarkers  (4)
  • Dissolved organic matter  (2)
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  • 1
    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2019. This is the author's version of the work. It is posted here by permission of Elsevier Ltd. for personal use, not for redistribution. The definitive version was published in Geochimica et Cosmochimica Acta 244 (2019): 216-228, doi:10.1016/j.gca.2018.10.012.
    Description: Mountain glaciers store dissolved organic carbon (DOC) that can be exported to river networks and subsequently respired to CO2. Despite this potential importance within the global carbon cycle, the seasonal variability and downstream transport of glacier-derived DOC in mountainous river basins remains largely unknown. To provide novel insight, here we present DOC concentrations and molecular-level dissolved organic matter (DOM) compositions from 22 nested, glaciated catchments (1.4 – 81.8 % glacier cover by area) in the Upper Ganges Basin, Western Himalaya over the course of the Indian summer monsoon (ISM) in 2014. Aliphatic and peptide-like compounds were abundant in glaciated headwaters but were overprinted by soil-derived phenolic, polyphenolic and condensed aromatic material as DOC concentrations increase moving downstream. Across the basin, DOC concentrations and soil-derived compound class contributions decreased sharply from pre- to post-ISM, implying increased relative contribution of glaciated headwater signals as the monsoon progresses. Incubation experiments further revealed a strong compositional control on the fraction of bioavailable DOC (BDOC), with glacier-derived DOC exhibiting the highest bioavailability. We hypothesize that short-term (i.e. in the coming decades) increases in glacier melt flux driven by climate change will further bias exported DOM toward an aliphatic-rich, bioavailable signal, especially during the ISM and post-ISM seasons. In contrast, eventual decreases in glacier melt flux due to mass loss will likely lead to more a soil-like DOM composition and lower bioavailability of exported DOC in the long term.
    Description: We thank Britta Voss (WHOI) for assisting with sample collection; Travis Drake (FSU), and Ekaterina Bulygina (Woods Hole Research Center) for laboratory assistance; and the NHMFL ICR user program (NSF-DMR-1157490) for aiding in data acquisition and analysis. This study was partly supported by NSF-DEB-1145932 to R.G.M.S. J.D.H. was partially supported by the NSF Graduate Research Fellowship Program under grant number 2012126152, with additional support in the form of travel grants awarded by the MIT Houghten Fund and NHMFL. All data used in this study are available in the Supporting Information Tables S1 and S2.
    Keywords: Dissolved organic matter ; Eco-hydrology ; Glaciers ; Himalaya ; Monsoon
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 2
    Publication Date: 2022-05-26
    Description: Author Posting. © American Geophysical Union, 2014. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geophysical Research Letters 41 (2014): 6420–6427, doi:10.1002/2014GL061328.
    Description: Rivers carry organic molecules derived from terrestrial vegetation to sedimentary deposits in lakes and oceans, storing information about past climate and erosion, as well as representing a component of the carbon cycle. It is anticipated that sourcing of organic matter may not be uniform across catchments with substantial environmental variability in topography, vegetation zones, and climate. Here we analyze plant leaf wax biomarkers in transit in the Madre de Dios River (Peru), which drains a forested catchment across 4.5 km of elevation from the tropical montane forests of the Andes down into the rainforests of Amazonia. We find that the hydrogen isotopic composition of leaf wax molecules (specifically the C28 n-alkanoic acid) carried by this tropical mountain river largely records the elevation gradient defined by the isotopic composition of precipitation, and this supports the general interpretation of these biomarkers as proxy recorders of catchment conditions. However, we also find that leaf wax isotopic composition varies with river flow regime over storm and seasonal timescales, which could in some cases be quantitatively significant relative to changes in the isotopic composition of precipitation in the past. Our results inform on the sourcing and transport of material by a major tributary of the Amazon River and contribute to the spatial interpretation of sedimentary records of past climate using the leaf wax proxy.
    Description: This work was supported by funding from the U.S. National Science Foundation award 1227192 to A.J.W. and S.J.F. V.G. was supported by the U.S. National Science Foundation award OCE-0928582.
    Description: 2015-03-23
    Keywords: Hydrogen isotopes ; Biomarkers ; Fluvial transport ; Erosion ; Paleoclimate ; Amazon
    Repository Name: Woods Hole Open Access Server
    Type: Article
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    Format: application/vnd.ms-excel
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  • 3
    Publication Date: 2022-05-26
    Description: © The Author(s), 2016. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Frontiers in Earth Science 4 (2016): 77, doi:10.3389/feart.2016.00077.
    Description: Arctic deltas are dynamic and vulnerable regions that play a key role in land-ocean interactions and the global carbon cycle. Delta lakes may provide valuable historical records of the quality and quantity of fluvial fluxes, parameters that are challenging to investigate in these remote regions. Here we study lakes from across the Mackenzie Delta, Arctic Canada, that receive fluvial sediments from the Mackenzie River when spring flood water levels rise above natural levees. We compare downcore lake sediments with suspended sediments collected during the spring flood, using bulk (% organic carbon, % total nitrogen, δ13C, Δ14C) and molecular organic geochemistry (lignin, leaf waxes). High-resolution age models (137Cs, 210Pb) of downcore lake sediment records (n = 11) along with lamina counting on high-resolution radiographs show sediment deposition frequencies ranging between annually to every 15 years. Down-core geochemical variability in a representative delta lake sediment core is consistent with historical variability in spring flood hydrology (variability in peak discharge, ice jamming, peak water levels). Comparison with earlier published Mackenzie River depth profiles shows that (i) lake sediments reflect the riverine surface suspended load, and (ii) hydrodynamic sorting patterns related to spring flood characteristics are reflected in the lake sediments. Bulk and molecular geochemistry of suspended particulate matter from the spring flood peak and lake sediments are relatively similar showing a mixture of modern higher-plant derived material, older terrestrial permafrost material, and old rock-derived material. This suggests that deltaic lake sedimentary records hold great promise as recorders of past (century-scale) riverine fluxes and may prove instrumental in shedding light on past behavior of arctic rivers, as well as how they respond to a changing climate.
    Description: Funding was provided by the US National Science Foundation as part of the Arctic Great Rivers Observatory (NSF-0732522 and NSF-1107774), as well as the Netherlands Organization for Scientific Research (Rubicon #825.10.022, and Veni #863.12.004). Additional funding for the lake coring was provided from WHOI through its Ocean and Climate Change Institute.
    Keywords: Lignin ; Biomarkers ; Mackenzie River ; Carbon isotopes ; Lake sediments
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 4
    Publication Date: 2022-05-26
    Description: © The Author(s), 2017. This is the author's version of the work. It is posted here under a nonexclusive, irrevocable, paid-up, worldwide license granted to WHOI. It is made available for personal use, not for redistribution. The definitive version was published in Chemical Geology 466 (2017): 454-465, doi:10.1016/j.chemgeo.2017.06.034.
    Description: We present dissolved organic carbon (DOC) concentrations, particulate organic matter (POM) composition (δ13C, δ15N, ∆14C, N/C), and particulate glycerol dialkyl glycerol tetraether (GDGT) distributions from a 34-month time-series near the mouth of the Congo River. An end-member mixing model using δ13C and N/C indicates that exported POM is consistently dominated by C3 rainforest soil sources, with increasing contribution from C3 vegetation and decreasing contribution from phytoplankton at high discharge. Large C4 inputs are never observed despite covering ≈ 13 % of the catchment. Low and variable ∆14C values during 2011 [annual mean = (-148 ± 82) ‰], when discharge from left-bank tributaries located in the southern hemisphere reached record lows, likely reflect a bias toward pre-aged POM derived from the Cuvette Congolaise swamp forest. In contrast, ∆14C values were stable near -50 ‰ between January and June 2013, when left-bank discharge was highest. We suggest that headwater POM is replaced and/or diluted by C3 vegetation and pre-aged soils during transit through the Cuvette Congolaise, whereas left-bank tributaries export significantly less pre-aged material. GDGT distributions provide further evidence for seasonal and inter-annual variability in soil provenance. The cyclization of branched tetraethers and the GDGT-0 to crenarchaeol ratio are positively correlated with discharge (r ≥ 0.70; p-value ≤ 4.3×10-5) due to the incorporation of swamp-forest soils when discharge from right-bank tributaries located in the northern hemisphere is high. Both metrics reach record lows during 2013, supporting our interpretation of increased left-bank contribution at this time. We conclude that hydrologic variability is a major control of POM provenance in the Congo River Basin and that tropical wetlands can be a significant POM source despite their small geographic coverage.
    Description: J.D.H. was supported by the NSF Graduate Research Fellowship Program under grant number 2012126152; E.S. was supported by the DFG Research Center/Cluster of Excellence “The Ocean in the Earth System” at MARUM – Center for Environmental Sciences; V.V.G. was partly supported by the US National Science Foundation, grants OCE-0851015 and OCE-0928582; R.G.M.S. was partly supported by the US National Science Foundation, grants OCE-0851101, OCE-1333157, and OCE-1464396; and T.I.E. was partly supported by the Swiss National Science Foundation (SNF Grant No. 200021_140850).
    Keywords: Biomarkers ; Congo River ; GDGTs ; Particulate Organic Matter ; Radiocarbon
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 5
    Publication Date: 2022-05-26
    Description: © The Author(s), 2017. This is the author's version of the work. It is posted here under a nonexclusive, irrevocable, paid-up, worldwide license granted to WHOI. It is made available for personal use, not for redistribution. The definitive version was published in Earth and Planetary Science Letters 478 (2017): 89-101, doi:10.1016/j.epsl.2017.08.013.
    Description: Climate has been proposed to control both the rate of terrestrial silicate weathering and the export rate of associated sediments and terrestrial organic carbon to river-dominated margins – and thus the rate of sequestration of atmospheric CO2 in the coastal ocean – over glacial-interglacial timescales. Focused on the Ganges-Brahmaputra rivers, this study presents records of post-glacial changes in basin-scale Indian summer monsoon intensity and vegetation composition based on stable hydrogen (δD) and carbon (δ13C) isotopic compositions of terrestrial plant wax compounds preserved in the channel-levee system of the Bengal Fan. It then explores the role of these changes in controlling the provenance and degree of chemical weathering of sediments exported by these rivers, and the potential climate feedbacks through organic-carbon burial in the Bengal Fan. An observed 40‰ shift in δD and a 3–4‰ shift in both bulk organic-carbon and plant-wax δ13C values between the late glacial and mid-Holocene, followed by a return to more intermediate values during the late Holocene, correlates well with regional post-glacial paleoclimate records. Sediment provenance proxies (Sr, Nd isotopic compositions) reveal that these changes likely coincided with a subtle focusing of erosion on the southern flank of the Himalayan range during periods of greater monsoon strength and enhanced sediment discharge. However, grain-size-normalized organic-carbon concentrations in the Bengal Fan remained constant through time, despite order-of-magnitude level changes in catchment-scale monsoon precipitation and enhanced chemical weathering (recorded as a gradual increase in K/Si* and detrital carbonate content, and decrease in H2O+/Si*, proxies) throughout the study period. These findings demonstrate a partial decoupling of climate change and silicate weathering during the Holocene and that marine organic-carbon sequestration rates primary reflect rates of physical erosion and sediment export as modulated by climatic changes. Together, these results reveal the magnitude of climate changes within the Ganges-Brahmaputra basin following deglaciation and a closer coupling of monsoon strength with OC burial than with silicate weathering on millennial timescales.
    Description: This work was supported by the National Science Foundation [grant numbers OCE-1333826 and OCE-1333387].
    Keywords: Indian Monsoon ; Bengal Fan ; Paleoclimate ; Sediment Provenance ; Biomarkers ; Stable Isotopes
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 6
    Publication Date: 2022-10-26
    Description: Author Posting. © American Geophysical Union, 2021. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research: Biogeosciences 126(7), (2021): e2020JG005977, https://doi.org/10.1029/2020JG005977.
    Description: Increasing Arctic temperatures are thawing permafrost soils and liberating ancient organic matter, but the fate of this material remains unclear. Thawing of permafrost releases dissolved organic matter (DOM) into fluvial networks. Unfortunately, tracking this material in Arctic rivers such as the Kolyma River in Siberia has proven challenging due to its high biodegradability. Here, we evaluate late summer abruptly thawed yedoma permafrost dissolved organic carbon (DOC) inputs from Duvannyi Yar. We implemented ultrahigh-resolution mass spectrometry alongside ramped pyrolysis oxidation (RPO) and isotopic analyses. These approaches offer insight into DOM chemical composition and DOC radiocarbon values of thermochemical components for a permafrost thaw stream, the Kolyma River, and their biodegraded counterparts (n = 4). The highly aliphatic molecular formula found in undegraded permafrost DOM contrasted with the comparatively aliphatic-poor formula of Kolyma River DOM, represented by an 8.9% and 2.6% relative abundance, respectively, suggesting minimal inputs of undegraded permafrost DOM in the river. RPO radiocarbon fractions of Kolyma River DOC exhibited no “hidden” aged component indicative of permafrost influence. Thermostability analyses suggested that there was limited biodegraded permafrost DOC in the Kolyma River, in part determined by the formation of high-activation energy (thermally stable) biodegradation components in permafrost DOM that were lacking in the Kolyma River. A mixing model based on thermostability and radiocarbon allowed us to estimate a maximum input of between 0.8% and 7.7% of this Pleistocene-aged permafrost to the Kolyma River DOC. Ultimately, our findings highlight that export of modern terrestrial DOC currently overwhelms any permafrost DOC inputs in the Kolyma River.
    Description: This work was funded by NSF grants ANT-1203885 and PLR-1500169 to R.G.M.S. The work was also supported by the National Science Foundation Division of Chemistry through DMR-1644779 and the State of Florida.
    Description: 2022-01-09
    Keywords: Permafrost ; Dissolved organic carbon ; Dissolved organic matter ; FT-ICR MS ; Ramped pyrolysis oxidation ; Arctic
    Repository Name: Woods Hole Open Access Server
    Type: Article
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