Abstract
The Arctic is warming at a rate twice that of other global ecosystems and changing climate conditions in the Arctic are mobilizing long frozen permafrost stores of organic carbon. In ice-rich regions, permafrost thaw on sloping terrain can cause land subsidence, and the development of thaw-driven mass wasting. The Peel Plateau, Northwest Territories, Canada has extensive thaw-driven landslides called retrogressive thaw slumps that are exposing early Holocene age paleo-thaw layers and Pleistocene age glaciogenic material deposited by the Laurentide Ice Sheet. This study aimed to see if unique retrogressive thaw slump derived permafrost inputs could be readily observed in streams across six diverse thermokarst features via optical and ultrahigh-resolution mass spectrometry. Aquatic samples from water draining thermokarst slump features, and downstream of thermokarst inputs exhibited higher dissolved organic carbon concentrations and lower aromaticity as evidenced by optical parameters (e.g. declining SUVA254, increasing S275-295) and FT-ICR MS metrics (e.g. lower AImod and nominal oxidation state of carbon) versus upstream of thermokarst impacts. Increases in the relative abundances of assigned heteroatomic molecular formulae (e.g. CHON, CHOS, CHONS) were also greater within and downstream of thermokarst features. The unique molecular formulae present in permafrost thermokarst inputs were determined (n = 1844) and subsequently tracked downstream. These permafrost marker formulae were enriched in aliphatics and H/C, as well as heteroatoms and exhibited low aromaticity. A portion of the unique molecular fingerprint persisted downstream, highlighting the potential to not only assess thermokarst inputs but also to follow these inputs and their fate downstream throughout the aquatic network.
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Data availability
All molecular formulae documented by the FT-ICR MS are available in the OSF database at https://osf.io/4kvys/ with the title: P19786_Tracing Permafrost Thaw DOM on the Peel Plateau, Canada.
Change history
13 January 2024
A Correction to this paper has been published: https://doi.org/10.1007/s10533-023-01114-y
References
Abbott BW, Larouche JR, Jones JB, Bowden WB, Balser AW (2014) Elevated dissolved organic carbon biodegradability from thawing and collapsing permafrost. J Geophys Res Biogeosci 119(10):2049–2063. https://doi.org/10.1002/2014JG002678
Behnke MI, McClelland JW, Tank SE, Kellerman AM, Holmes RM, Haghipour N, Eglinton TI, Raymond PA, Suslova A, Zhulidov Av, Gurtovaya T, Zimov N, Zimov S, Mutter EA, Amos E, Spencer RGM (2021) Pan-Arctic Riverine Dissolved Organic Matter: Synchronous Molecular Stability Shifting Sources and Subsidies. Glob Biogeochem Cycles. https://doi.org/10.1029/2020GB006871
Biskaborn BK, Smith SL, Noetzli J, Matthes H, Vieira G, Streletskiy DA, Schoeneich P, Romanovsky VE, Lewkowicz AG, Abramov A, Allard M, Boike J, Cable WL, Christiansen HH, Delaloye R, Diekmann B, Drozdov D, Etzelmüller B, Grosse G, Lantuit H (2019) Permafrost is warming at a global scale. Nat Commun 10(1):264. https://doi.org/10.1038/s41467-018-08240-4
Bröder L, Keskitalo K, Zolkos S, Shakil S, Tank SE, Kokelj Sv, Tesi T, van Dongen BE, Haghipour N, Eglinton TI, Vonk JE (2021) Preferential export of permafrost-derived organic matter as retrogressive thaw slumping intensifies. Environ Res Lett. https://doi.org/10.1088/1748-9326/abee4b
Burn CR (1997) Cryostratigraphy, paleogeography, and climate change during the early Holocene warm interval, western Arctic coast. Can Can J Earth Sci 34(7):912–925. https://doi.org/10.1139/e17-076
Collins MJ, Bishop AN, Farrimond P (1995) Sorption by mineral surfaces: Rebirth of the classical condensation pathway for kerogen formation? Geochim Cosmochim Acta 59(11):2387–2391. https://doi.org/10.1016/0016-7037(95)00114-F
Corilo, Y. (2015). PetroOrg. Florida State University.
de Haan H, de Boer T (1987) Applicability of light absorbance and fluorescence as measures of concentration and molecular size of dissolved organic carbon in humic Lake Tjeukemeer. Water Res 21(6):731–734. https://doi.org/10.1016/0043-1354(87)90086-8
Dittmar T, Koch B, Hertkorn N, Kattner G (2008) A simple and efficient method for the solid-phase extraction of dissolved organic matter (SPE-DOM) from seawater. Limnol Oceanogr Methods. https://doi.org/10.4319/lom.2008.6.230
Drake TW, Guillemette F, Hemingway JD, Chanton JP, Podgorski DC, Zimov NS, Spencer RGM (2018) The Ephemeral Signature of Permafrost Carbon in an Arctic Fluvial Network. J Geophys Res Biogeosci 123(5):1475–1485. https://doi.org/10.1029/2017JG004311
Duk-Rodkin, A. (1992). Surficial Geology, Fort McPherson-Bell River, Yukon-Northwest Territories. https://doi.org/10.4095/184002
Dutta H, Dutta A (2016) The microbial aspect of climate change. Energy Ecol Environ 1(4):209–232. https://doi.org/10.1007/s40974-016-0034-7
Environment Canada (2015) Canadian Climate Normals 1981–2010 Station Data.
Green SA, Blough NV (1994) Optical absorption and fluorescence properties of chromophoric dissolved organic matter in natural waters. Limnol Oceanogr 39(8):1903–1916. https://doi.org/10.4319/lo.1994.39.8.1903
Gruber S (2012) Derivation and analysis of a high-resolution estimate of global permafrost zonation. Cryosphere 6(1):221–233. https://doi.org/10.5194/tc-6-221-2012
Helms JR, Stubbins A, Ritchie JD, Minor EC, Kieber DJ, Mopper K (2008) Absorption spectral slopes and slope ratios as indicators of molecular weight, source, and photobleaching of chromophoric dissolved organic matter. Limnol Oceanogr 53(3):955–969. https://doi.org/10.4319/lo.2008.53.3.0955
Hendrickson CL, Quinn JP, Kaiser NK, Smith DF, Blakney GT, Chen T, Marshall AG, Weisbrod CR, Beu SC (2015) 21 Tesla Fourier Transform Ion Cyclotron Resonance Mass Spectrometer: A National Resource for Ultrahigh Resolution Mass Analysis. J Am Soc Mass Spectrom 26(9):1626–1632. https://doi.org/10.1007/s13361-015-1182-2
Kassambara AM, Mundt F (2017) Factoextra: Extract and visualize the results of multivariate data analyses. R package version 1(4)
Kawahigashi M, Kaiser K, Rodionov A, Guggenberger G (2006) Sorption of dissolved organic matter by mineral soils of the Siberian forest tundra. Glob Change Biol 12(10):1868–1877. https://doi.org/10.1111/j.1365-2486.2006.01203.x
Kellerman AM, Guillemette F, Podgorski DC, Aiken GR, Butler KD, Spencer RGM (2018) Unifying Concepts Linking Dissolved Organic Matter Composition to Persistence in Aquatic Ecosystems. Environ Sci Technol 52(5):2538–2548. https://doi.org/10.1021/acs.est.7b05513
Kokelj SV, Tunnicliffe J, Lacelle D, Lantz TC, Chin KS, Fraser R (2015) Increased precipitation drives mega slump development and destabilization of ice-rich permafrost terrain, northwestern Canada. Global Planet Change 129:56–68. https://doi.org/10.1016/j.gloplacha.2015.02.008
Kokelj SV, Kokoszka J, van der Sluijs J, Rudy ACA, Tunnicliffe J, Shakil S, Tank SE, Zolkos S (2021) Thaw-driven mass wasting couples slopes with downstream systems, and effects propagate through Arctic drainage networks. Cryosphere 15(7):3059–3081. https://doi.org/10.5194/tc-15-3059-2021
Kokelj Sv, Tunnicliffe JF, Lacelle D (2017) The Peel Plateau of Northwestern Canada: An Ice-Rich Hummocky Moraine Landscape in Transition, pp. 109–122. https://doi.org/10.1007/978-3-319-44595-3_7
Kurek MR, Stubbins A, Drake TW, Moura JMS, Holmes RM, Osterholz H, Dittmar T, Peucker-Ehrenbrink B, Mitsuya M, Spencer RGM (2021) Drivers of Organic Molecular Signatures in the Amazon River. Glob Biogeochem Cycles. https://doi.org/10.1029/2021GB006938
Kurek MR, Frey KE, Guillemette F, Podgorski DC, Townsend-Small A, Arp CD, Kellerman AM, Spencer RGM (2022a) Trapped Under Ice: Spatial and Seasonal Dynamics of Dissolved Organic Matter Composition in Tundra Lakes. J Geophys Res Biogeosci. https://doi.org/10.1029/2021JG006578
Kurek MR, Stubbins A, Drake TW, Dittmar TMS, Moura J, Holmes RM, Osterholz H, Six J, Wabakanghanzi JN, Dinga B, Mitsuya M, Spencer RGM (2022b) Organic molecular signatures of the Congo river and comparison to the Amazon. Glob Biogeochem Cycles. https://doi.org/10.1029/2022GB007301
Kurek MR, Garcia-Tigreros F, Wickland KP, Frey KE, Dornblaser MM, Striegl RG, Niles SF, McKenna AM, Aukes PJK, Kyzivat ED, Wang C, Pavelsky TM, Smith LC, Schiff SL, Butman D, Spencer RGM (2023) Hydrologic and Landscape Controls on Dissolved Organic Matter Composition Across Western North American Arctic Lakes. Glob Biogeochem Cycles. https://doi.org/10.1029/2022GB007495
Lacelle D, Lauriol B, Zazula G, Ghaleb B, Utting N, Clark ID (2013) Timing of advance and basal condition of the Laurentide Ice Sheet during the last glacial maximum in the Richardson Mountains. NWT Q Res 80(2):274–283. https://doi.org/10.1016/j.yqres.2013.06.001
LaRowe DE, van Cappellen P (2011) Degradation of natural organic matter: A thermodynamic analysis. Geochim Cosmochim Acta 75(8):2030–2042. https://doi.org/10.1016/j.gca.2011.01.020
Leewis M-C, Berlemont R, Podgorski DC, Srinivas A, Zito P, Spencer RGM, McFarland J, Douglas TA, Conaway CH, Waldrop M, Mackelprang R (2020) Life at the Frozen Limit: Microbial Carbon Metabolism Across a Late Pleistocene Permafrost Chronosequence. Front Microbiol. https://doi.org/10.3389/fmicb.2020.01753
Lewkowicz AG, Way RG (2019) Extremes of summer climate trigger thousands of thermokarst landslides in a High Arctic environment. Nat Commun 10(1):1329. https://doi.org/10.1038/s41467-019-09314-7
Littlefair CA, Tank SE (2018) Biodegradability of Thermokarst Carbon in a Till-Associated, Glacial Margin Landscape: The Case of the Peel Plateau, NWT. Can J Geophys Res Biogeosci 123(10):3293–3307. https://doi.org/10.1029/2018JG004461
Littlefair CA, Tank SE, Kokelj Sv (2017) Retrogressive thaw slumps temper dissolved organic carbon delivery to streams of the Peel Plateau, NWT. Can Biogeosci 14(23):5487–5505. https://doi.org/10.5194/bg-14-5487-2017
Mann PJ, Davydova A, Zimov N, Spencer RGM, Davydov S, Bulygina E, Zimov S, Holmes RM (2012) Controls on the composition and lability of dissolved organic matter in Siberia’s Kolyma River basin. J Geophys Res Biogeosci. https://doi.org/10.1029/2011JG001798
Mooshammer M, Wanek W, Hämmerle I, Fuchslueger L, Hofhansl F, Knoltsch A, Schnecker J, Takriti M, Watzka M, Wild B, Keiblinger KM, Zechmeister-Boltenstern S, Richter A (2014) Adjustment of microbial nitrogen use efficiency to carbon:nitrogen imbalances regulates soil nitrogen cycling. Nat Commun 5(1):3694. https://doi.org/10.1038/ncomms4694
Murphy KR, Stedmon CA, Graeber D, Bro R (2013) Fluorescence spectroscopy and multi-way techniques. PARAFAC. Anal Methods. https://doi.org/10.1039/c3ay41160e
Obu J (2021) How Much of the Earth’s Surface is Underlain by Permafrost? J Geophys Res Earth Surface. https://doi.org/10.1029/2021JF006123
Olefeldt D, Roulet NT (2012) Effects of permafrost and hydrology on the composition and transport of dissolved organic carbon in a subarctic peatland complex. J Geophys Res Biogeosci. https://doi.org/10.1029/2011JG001819
O’Neill HB, Burn CR, Kokelj SV, Lantz TC (2015) ‘Warm’ Tundra: Atmospheric and Near-Surface Ground Temperature Inversions Across an Alpine Treeline in Continuous Permafrost, Western Arctic. Can Permafrost Periglacial Processes 26(2):103–118. https://doi.org/10.1002/ppp.1838
Peter S, Shen Y, Kaiser K, Benner R, Durisch-Kaiser E (2012) Bioavailability and diagenetic state of dissolved organic matter in riparian groundwater. J Geophys Res Biogeosci. https://doi.org/10.1029/2012JG002072
Peuravuori J, Pihlaja K (1997) Molecular size distribution and spectroscopic properties of aquatic humic substances. Anal Chim Acta 337(2):133–149. https://doi.org/10.1016/S0003-2670(96)00412-6
R Core Team (2019) A language and environment for statistical computing. R Foundation for Statistical Computing (https://www.R-project.org/)
Richter-Menge J, Druckenmiller ML, Jeffries M (2019) Arctic Report Card 2019
Rogers JA, Galy V, Kellerman AM, Chanton JP, Zimov N, Spencer RGM (2021) Limited Presence of Permafrost Dissolved Organic Matter in the Kolyma River, Siberia Revealed by Ramped Oxidation. J Geophys Res Biogeosci. https://doi.org/10.1029/2020JG005977
Šantl-Temkiv T, Finster K, Dittmar T, Hansen BM, Thyrhaug R, Nielsen NW, Karlson UG (2013) Hailstones: A Window into the Microbial and Chemical Inventory of a Storm Cloud. PLoS ONE 8(1):e53550. https://doi.org/10.1371/journal.pone.0053550
Schmidt F, Elvert M, Koch BP, Witt M, Hinrichs K-U (2009) Molecular characterization of dissolved organic matter in pore water of continental shelf sediments. Geochim Cosmochim Acta 73(11):3337–3358. https://doi.org/10.1016/j.gca.2009.03.008
Schuur E, Bockham J, Canadell J (2008) Vulnerability of Permafrost Carbon to Climate Change: Implications for the Global Carbon Cycle. Bioscience 58:701
Shakil S, Tank SE, Kokelj SV, Vonk JE, Zolkos S (2020) Particulate dominance of organic carbon mobilization from thaw slumps on the Peel Plateau, NT: Quantification and implications for stream systems and permafrost carbon release. Environ Res Lett 15(11):114019. https://doi.org/10.1088/1748-9326/abac36
Sinsabaugh RL, Turner BL, Talbot JM, Waring BG, Powers JS, Kuske CR, Moorhead DL, Follstad Shah JJ (2016) Stoichiometry of microbial carbon use efficiency in soils. Ecol Monogr 86(2):172–189. https://doi.org/10.1890/15-2110.1
Sistla SA, Asao S, Schimel JP (2012) Detecting microbial N-limitation in tussock tundra soil: Implications for Arctic soil organic carbon cycling. Soil Biol Biochem 55:78–84. https://doi.org/10.1016/j.soilbio.2012.06.010
Sleighter RL, Hatcher PG (2008) Molecular characterization of dissolved organic matter (DOM) along a river to ocean transect of the lower Chesapeake Bay by ultrahigh resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Mar Chem 110(3–4):140–152. https://doi.org/10.1016/j.marchem.2008.04.008
Smith DF, Podgorski DC, Rodgers RP, Blakney GT, Hendrickson CL (2018) 21 Tesla FT-ICR Mass Spectrometer for Ultrahigh-Resolution Analysis of Complex Organic Mixtures. Anal Chem 90(3):2041–2047. https://doi.org/10.1021/acs.analchem.7b04159
Spencer RGM, Baker A, Ahad JME, Cowie GL, Ganeshram R, Upstill-Goddard RC, Uher G (2007) Discriminatory classification of natural and anthropogenic waters in two U.K. estuaries. Sci Total Environ 373(1):305–323. https://doi.org/10.1016/j.scitotenv.2006.10.052
Spencer RGM, Butler KD, Aiken GR (2012) Dissolved organic carbon and chromophoric dissolved organic matter properties of rivers in the USA. J Geophys Res Biogeosci. https://doi.org/10.1029/2011JG001928
Spencer RGM, Mann PJ, Dittmar T, Eglinton TI, McIntyre C, Holmes RM, Zimov N, Stubbins A (2015) Detecting the signature of permafrost thaw in Arctic rivers. Geophys Res Lett 42(8):2830–2835. https://doi.org/10.1002/2015GL063498
Subdiaga E, Harir M, Orsetti S, Hertkorn N, Schmitt-Kopplin P, Haderlein SB (2020) Preferential Sorption of Tannins at Aluminum Oxide Affects the Electron Exchange Capacities of Dissolved and Sorbed Humic Acid Fractions. Environ Sci Technol 54(3):1837–1847. https://doi.org/10.1021/acs.est.9b04733
Textor SR, Wickland KP, Podgorski DC, Johnston SE, Spencer RGM (2019) Dissolved Organic Carbon Turnover in Permafrost-Influenced Watersheds of Interior Alaska: Molecular Insights and the Priming Effect. Front Earth Sci. https://doi.org/10.3389/feart.2019.00275
The Physical Science Basis Summary for Policymakers Working Group I contribution to the Sixth Assessment Report of the Intergovernmental Panel on Climate Change. (2021).
van der Sluijs J (2023) Allometric scaling of retrogressive thaw slumps. Eu Geosci Union: Cryosphere 17(11):4511–4533. https://doi.org/10.5194/tc-17-4511-2023
Vaughn DR, Kellerman AM, Wickland KP, Striegl RG, Podgorski DC, Hawkings JR, Nienhuis JH, Dornblaser MM, Stets EG, Spencer RGM (2021) Anthropogenic landcover impacts fluvial dissolved organic matter composition in the Upper Mississippi River Basin. Biogeochemistry. https://doi.org/10.1007/s10533-021-00852-1
Vonk JE, Mann PJ, Davydov S, Davydova A, Spencer RGM, Schade J, Sobczak WV, Zimov N, Zimov S, Bulygina E, Eglinton TI, Holmes RM (2013) High biolability of ancient permafrost carbon upon thaw. Geophys Res Lett 40(11):2689–2693. https://doi.org/10.1002/grl.50348
Vonk JE, Tank SE, Bowden WB, Laurion I, Vincent WF, Alekseychik P, Amyot M, Billet MF, Canário J, Cory RM, Deshpande BN, Helbig M, Jammet M, Karlsson J, Larouche J, Macmillan G, Rautio M, Walter Anthony KM, Wickland KP (2015) Reviews and syntheses: Effects of permafrost thaw on Arctic aquatic ecosystems. In Biogeosciences (Vol. 12, Issue 23, pp. 7129–7167). Copernicus GmbH. 10.5194/bg-12-7129-2015
Vonk JE, Tank SE, Mann PJ, Spencer RGM, Treat CC, Striegl RG, Abbott BW, Wickland KP (2015b) Biodegradability of dissolved organic carbon in permafrost soils and aquatic systems: A meta-analysis. Biogeosciences 12(23):6915–6930. https://doi.org/10.5194/bg-12-6915-2015
Wagner S, Riedel T, Niggemann J, Vähätalo AV, Dittmar T, Jaffé R (2015) Linking the Molecular Signature of Heteroatomic Dissolved Organic Matter to Watershed Characteristics in World Rivers. Environ Sci Technol 49(23):13798–13806. https://doi.org/10.1021/acs.est.5b00525
Ward CP, Nalven SG, Crump BC, Kling GW, Cory RM (2017) Photochemical alteration of organic carbon draining permafrost soils shifts microbial metabolic pathways and stimulates respiration. Nat Commun. https://doi.org/10.1038/s41467-017-00759-2
Weishaar JL, Aiken GR, Bergamaschi BA, Fram MS, Fujii R, Mopper K (2003) Evaluation of Specific Ultraviolet Absorbance as an Indicator of the Chemical Composition and Reactivity of Dissolved Organic Carbon. Environ Sci Technol 37(20):4702–4708. https://doi.org/10.1021/es030360x
Wickham H (2016) ggplot2: elegant graphics for data analysis. springer.
Wild B, Schnecker J, Knoltsch A, Takriti M, Mooshammer M, Gentsch N, Mikutta R, Alves RJE, Gittel A, Lashchinskiy N, Richter A (2015) Microbial nitrogen dynamics in organic and mineral soil horizons along a latitudinal transect in western Siberia. Glob Biogeochem Cycles 29(5):567–582. https://doi.org/10.1002/2015GB005084
Zolkos S, Tank SE (2019) Permafrost Geochemistry and Retrogressive Thaw Slump Morphology (Peel Plateau, Canada)
Zolkos S, Tank SE, Kokelj SV (2018) Mineral Weathering and the Permafrost Carbon-Climate Feedback. Geophys Res Lett 45(18):9623–9632. https://doi.org/10.1029/2018GL078748
Zolkos S, Tank SE, Striegl RG, Kokelj S, v. (2019) Thermokarst Effects on Carbon Dioxide and Methane Fluxes in Streams on the Peel Plateau (NWT, Canada). J Geophys Res Biogeosci 124(7):1781–1798. https://doi.org/10.1029/2019JG005038
Acknowledgements
Thank you to all funding partners including Polar Continental Shelf Program grant number 657-21 for helicopter support, and NSERC (Natural Sciences and Engineering Council of Canada; grants RGPIN-2019-05524 and RGPNS-2019-444873), UAlberta North, POLAR Canada (Northern Scientific Training Program), and ArcticNet Canada (grant P13). Thank you to all of the field support during sample collection including A. Koe, and the Tetlit Gwich'in Renewable Resource Council in Fort McPherson. A portion of this work was conducted at the National High Magnetic Field Laboratory ICR User Facility, which is funded by the National Science Foundation Division of Chemistry through DMR-1644779 and the State of Florida. The authors thank all the helpful researchers at the NHMFL, ICR Program who enabled data acquisition and processing. Thank you to Dr. Jacob Carstens for assistance in creating Figures 2, 3, 4 and 5. The authors appreciate the guidance from our lab group members Amy Holt and Sommer Starr during data processing.
Funding
Polar Continental Shelf Program grant number 657-21 for helicopter support, and NSERC (Natural Sciences and Engineering Council of Canada; grants RGPIN-2019-05524 and RGPNS-2019-444873), UAlberta North, POLAR Canada (Northern Scientific Training Program), and ArcticNet Canada (grant P13). A portion of this work was conducted at the National High Magnetic Field Laboratory ICR User Facility, which is funded by the National Science Foundation Division of Chemistry through DMR-1644779 and the State of Florida.
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10533_2023_1101_MOESM1_ESM.xlsx
Supplementary file1 List of all formula present, and their formula class, for each group of sample types: upstream common, within-slump common, within-slump unique, and within-slump unique in downstream (XLSX 319 KB)
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Moore, M.R.N., Tank, S.E., Kurek, M.R. et al. Ultrahigh resolution dissolved organic matter characterization reveals distinct permafrost characteristics on the Peel Plateau, Canada. Biogeochemistry 167, 99–117 (2024). https://doi.org/10.1007/s10533-023-01101-3
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DOI: https://doi.org/10.1007/s10533-023-01101-3