TY - JOUR T1 - Temporal deconvolution of vascular plant-derived fatty acids exported from terrestrial watersheds JF - Geochimica et Cosmochimica Acta Y1 - 2019 A1 - Vonk, Jorien E. A1 - Drenzek, Nicholas J. A1 - Hughen, Konrad A. A1 - Stanley, Rachel H.R. A1 - McIntyre, Cameron A1 - çon, Daniel B. A1 - Giosan, Liviu A1 - Southon, John R. A1 - Santos, Guaciara M. A1 - Druffel, Ellen R.M. A1 - Andersson, August A. A1 - öld, Martin A1 - Eglinton, Timothy I. KW - british-columbia KW - CARIACO BASIN KW - compound-specific radiocarbon KW - MACKENZIE DELTA KW - marine-sediments KW - odp leg 169s KW - saanich inlet KW - SANTA-MONICA BASIN KW - SOIL ORGANIC-MATTER KW - TROPICAL VEGETATION AB - Relatively little is known about the amount of time that lapses between the photosynthetic fixation of carbon by vascular land plants and its incorporation into the marine sedimentary record, yet the dynamics of terrestrial carbon sequestration have important implications for the carbon cycle. Vascular plant carbon may encounter multiple potential intermediate storage pools and transport trajectories, and the age of vascular plant carbon accumulating in marine sediments will reflect these different pre-depositional histories. Here, we examine down-core C-14 profiles of higher plant leaf wax-derived fatty acids isolated from high fidelity sedimentary sequences spanning the so-called "bomb-spike", and encompassing a ca. 60-degree latitudinal gradient from tropical (Cariaco Basin), temperate (Saanich Inlet), and polar (Mackenzie Delta) watersheds to constrain integrated vascular plant carbon storage/transport times ("residence times"). Using a modeling framework, we find that, in addition to a "young" (conditionally defined as < 50 y) carbon pool, an old pool of compounds comprises 49 to 78 % of the fractional contribution of organic carbon (OC) and exhibits variable ages reflective of the environmental setting. For the Mackenzie Delta sediments, we find a mean age of the old pool of 28 ky (+/- 9.4, standard deviation), indicating extensive pre-aging in permafrost soils, whereas the old pools in Saanich Inlet and Cariaco Basin sediments are younger, 7.9 (+/- 5.0) and 2.4 (+/- 0.50) to 3.2 (+/- 0.54) ky, respectively, indicating less protracted storage in terrestrial reservoirs. The "young" pool showed clear annual contributions for Saanich Inlet and Mackenzie Delta sediments (comprising 24% and 16% of this pool, respectively), likely reflecting episodic transport of OC from steep hillside slopes surrounding Saanich Inlet and annual spring flood deposition in the Mackenzie Delta, respectively. Contributions of 5-10 year old OC to the Cariaco Basin show a short delay of OC inflow, potentially related to transport time to the offshore basin. Modeling results also indicate that the Mackenzie Delta has an influx of young but decadal material (20-30 years of age), pointing to the presence of an intermediate reservoir. Overall, these results show that a significant fraction of vascular plant C undergoes pre-aging in terrestrial reservoirs prior to accumulation in deltaic and marine sediments. The age distribution, reflecting both storage and transport times, likely depends on landscape-specific factors such as local topography, hydrographic characteristics, and mean annual temperature of the catchment, all of which affect the degree of soil buildup and preservation. We show that catchment-specific carbon residence times across landscapes can vary by an order of magnitude, with important implications both for carbon cycle studies and for the interpretation of molecular terrestrial paleoclimate records preserved in sedimentary sequences. VL - 244 UR - https://linkinghub.elsevier.com/retrieve/pii/S0016703718305702https://api.elsevier.com/content/article/PII:S0016703718305702?httpAccept=text/xmlhttps://api.elsevier.com/content/article/PII:S0016703718305702?httpAccept=text/plain ER - TY - JOUR T1 - Carbon geochemistry of plankton-dominated samples in the Laptev and East Siberian shelves: contrasts in suspended particle composition JF - Ocean Science Y1 - 2017 A1 - Tesi, Tommaso A1 - Geibel, Marc C. A1 - Pearce, Christof A1 - Panova, Elena A1 - Vonk, Jorien E. A1 - Karlsson, Emma A1 - Salvado, Joan A. A1 - Kruså, Martin A1 - Broder, Lisa A1 - Humborg, Christoph A1 - Semiletov, Igor A1 - Gustafsson, Örjan AB - Recent Arctic studies suggest that sea ice decline and permafrost thawing will affect phytoplankton dynamics and stimulate heterotrophic communities. However, in what way the plankton composition will change as the warming proceeds remains elusive. Here we investigate the chemical signature of the plankton-dominated fraction of particulate organic matter (POM) collected along the Siberian Shelf. POM (> 10 µm) samples were analysed using molecular biomarkers (CuO oxidation and IP25) and dual-carbon isotopes (δ13C and Δ14C). In addition, surface water chemical properties were integrated with the POM (> 10 µm) dataset to understand the link between plankton composition and environmental conditions. δ13C and Δ14C exhibited a large variability in the POM (> 10 µm) distribution while the content of terrestrial biomarkers in the POM was negligible. In the Laptev Sea (LS), δ13C and Δ14C of POM (> 10 µm) suggested a heterotrophic environment in which dissolved organic carbon (DOC) from the Lena River was the primary source of metabolisable carbon. Within the Lena plume, terrestrial DOC probably became part of the food web via bacteria uptake and subsequently transferred to relatively other heterotrophic communities (e.g. dinoflagellates). Moving eastwards toward the sea-ice-dominated East Siberian Sea (ESS), the system became progressively more autotrophic. Comparison between δ13C of POM (> 10 µm) samples and CO2aq concentrations revealed that the carbon isotope fractionation increased moving towards the easternmost and most productive stations. In a warming scenario characterised by enhanced terrestrial DOC release (thawing permafrost) and progressive sea ice decline, heterotrophic conditions might persist in the LS while the nutrient-rich Pacific inflow will likely stimulate greater primary productivity in the ESS. The contrasting trophic conditions will result in a sharp gradient in δ13C between the LS and ESS, similar to what is documented in our semi-synoptic study. VL - 13 UR - https://os.copernicus.org/articles/13/735/2017/ IS - 5 ER - TY - JOUR T1 - Arctic Deltaic Lake Sediments As Recorders of Fluvial Organic Matter Deposition Y1 - 2016 A1 - Vonk, Jorien E. A1 - Dickens, Angela F. A1 - Giosan, Liviu A1 - Hussain, Zainab A. A1 - Kim, Bokyung A1 - Zipper, Samuel C. A1 - Holmes, Robert M. A1 - Montluçon, Daniel B. A1 - Galy, Valier A1 - Eglinton, Timothy I. AB - 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, 13C, 14C) 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 behaviour of arctic rivers, as well as how they respond to a changing climate. VL - 4 SN - 2296-6463 UR - http://journal.frontiersin.org/article/10.3389/feart.2016.00077 ER - TY - JOUR T1 - Multimolecular tracers of terrestrial carbon transfer across the pan-Arctic: C-14 characteristics of sedimentary carbon components and their environmental controls JF - GLOBAL BIOGEOCHEMICAL CYCLES Y1 - 2015 A1 - Feng, Xiaojuan A1 - Gustafsson, Örjan A1 - Holmes, R. Max A1 - Vonk, Jorien E. A1 - van Dongen, Bart E. A1 - Semiletov, Igor P. A1 - Dudarev, Oleg V. A1 - Yunker, Mark B. A1 - Macdonald, Robie W. A1 - Wacker, Lukas A1 - Montluçon, Daniel B. A1 - Eglinton, Timothy I. AB - Distinguishing the sources, ages, and fate of various terrestrial organic carbon (OC) pools mobilized from heterogeneous Arctic landscapes is key to assessing climatic impacts on the fluvial release of carbon from permafrost. Through molecular C-14 measurements, including novel analyses of suberin- and/or cutin-derived diacids (DAs) and hydroxy fatty acids (FAs), we compared the radiocarbon characteristics of a comprehensive suite of terrestrial markers (including plant wax lipids, cutin, suberin, lignin, and hydroxy phenols) in the sedimentary particles from nine major arctic and subarctic rivers in order to establish a benchmark assessment of the mobilization patterns of terrestrial OC pools across the pan-Arctic. Terrestrial lipids, including suberin-derived longer-chain DAs (C-24,C-26,C-28), plant wax FAs (C(24,26,2)8), and n-alkanes (C-27,C-29,C-31), incorporated significant inputs of aged carbon, presumably from deeper soil horizons. Mobilization and translocation of these ``old{''} terrestrial carbon components was dependent on nonlinear processes associated with permafrost distributions. By contrast, shorter-chain (C-16,C-18) DAs and lignin phenols (as well as hydroxy phenols in rivers outside eastern Eurasian Arctic) were much more enriched in C-14, suggesting incorporation of relatively young carbon supplied by runoff processes from recent vegetation debris and surface layers. Furthermore, the radiocarbon content of terrestrial markers is heavily influenced by specific OC sources and degradation status. Overall, multitracer molecular C-14 analysis sheds new light on the mobilization of terrestrial OC from arctic watersheds. Our findings of distinct ages for various terrestrial carbon components may aid in elucidating fate of different terrestrial OC pools in the face of increasing arctic permafrost thaw. VL - 29 ER - TY - JOUR T1 - Preferential burial of permafrost-derived organic carbon in Siberian-Arctic shelf waters JF - JOURNAL OF GEOPHYSICAL RESEARCH-OCEANS Y1 - 2014 A1 - Vonk, Jorien E. A1 - Semiletov, Igor P. A1 - Dudarev, Oleg V. A1 - Eglinton, Timothy I. A1 - Andersson, August A1 - Shakhova, Natalia A1 - Charkin, Alexander A1 - Heim, Birgit A1 - Gustafsson, Örjan KW - biomarkers KW - carbon KW - permafrost KW - radiocarbon AB - The rapidly changing East Siberian Arctic Shelf (ESAS) receives large amounts of terrestrial organic carbon (OC) from coastal erosion and Russian-Arctic rivers. Climate warming increases thawing of coastal Ice Complex Deposits (ICD) and can change both the amount of released OC, as well as its propensity to be converted to greenhouse gases (fueling further global warming) or to be buried in coastal sediments. This study aimed to unravel the susceptibility to degradation, and transport and dispersal patterns of OC delivered to the ESAS. Bulk and molecular radiocarbon analyses on surface particulate matter (PM), sinking PM and underlying surface sediments illustrate the active release of old OC from coastal permafrost. Molecular tracers for recalcitrant soil OC showed ages of 3.4-13 C-14-ky in surface PM and 5.5-18 C-14-ky in surface sediments. The age difference of these markers between surface PM and surface sediments is larger (i) in regions with low OC accumulation rates, suggesting a weaker exchange between water column and sediments, and (ii) with increasing distance from the Lena River, suggesting preferential settling of fluvially derived old OC nearshore. A dual-carbon end-member mixing model showed that (i) contemporary terrestrial OC is dispersed mainly by horizontal transport while being subject to active degradation, (ii) marine OC is most affected by vertical transport and also actively degraded in the water column, and (iii) OC from ICD settles rapidly and dominates surface sediments. Preferential burial of ICD-OC released into ESAS coastal waters might therefore lower the suggested carbon cycle climate feedback from thawing ICD permafrost. VL - 119 ER -