@article {2921, title = {Climate control on terrestrial biospheric carbon turnover}, journal = {Proceedings of the National Academy of Sciences}, volume = {118}, year = {2021}, month = {Nov-02-2022}, pages = {e2011585118}, abstract = {Terrestrial vegetation and soils hold three times more carbon than the atmosphere. Much debate concerns how anthropogenic activity will perturb these surface reservoirs, potentially exacerbating ongoing changes to the climate system. Uncertainties specifically persist in extrapolating point-source observations to ecosystem-scale budgets and fluxes, which require consideration of vertical and lateral processes on multiple temporal and spatial scales. To explore controls on organic carbon (OC) turnover at the river basin scale, we present radiocarbon (C-14) ages on two groups of molecular tracers of plant-derived carbon-leaf-wax lipids and lignin phenols-from a globally distributed suite of rivers. We find significant negative relationships between the C-14 age of these biomarkers and mean annual temperature and precipitation. Moreover, riverine biospheric-carbon ages scale proportionally with basin-wide soil carbon turnover times and soil C-14 ages, implicating OC cycling within soils as a primary control on exported biomarker ages and revealing a broad distribution of soil OC reactivities. The ubiquitous occurrence of a long-lived soil OC pool suggests soil OC is globally vulnerable to perturbations by future temperature and precipitation increase. Scaling of riverine biospheric-carbon ages with soil OC turnover shows the former can constrain the sensitivity of carbon dynamics to environmental controls on broad spatial scales. Extracting this information from fluvially dominated sedimentary sequences may inform past variations in soil OC turnover in response to anthropogenic and/or climate perturbations. In turn, monitoring riverine OC composition may help detect future climate-change-induced perturbations of soil OC turnover and stocks.}, keywords = {Carbon cycle, carbon turnover times, fluvial carbon, plant biomarkers, radiocarbon}, issn = {0027-8424}, doi = {10.1073/pnas.2011585118}, url = {https://www.researchgate.net/publication/349357864_Climate_control_on_terrestrial_biospheric_carbon_turnover}, author = {Eglinton, Timothy I. and Galy, Valier V. and Hemingway, Jordon D. and Feng, Xiaojuan and Bao, Hongyan and Blattmann, Thomas M. and Dickens, Angela F. and Gies, Hannah and Giosan, Liviu and Haghipour, Negar and Hou, Pengfei and Lupker, Maarten and McIntyre, Cameron P. and Montlu{\c c}on, Daniel B. and Peucker-Ehrenbrink, Bernhard and Ponton, Camilo and Schefu{\ss}, Enno and Schwab, Melissa S. and Voss, Britta M. and Wacker, Lukas and Wu, Ying and Zhao, Meixun} } @article {2626, title = {Spatiotemporal Variation of the Quality, Origin, and Age of Particulate Organic Matter Transported by the Yangtze River (Changjiang)}, journal = {Journal of Geophysical Research: Biogeosciences}, volume = {123}, year = {2018}, month = {Jan-09-2018}, pages = {2908 - 2921}, abstract = {Information on the age dynamics of particulate organic matter (POM) in large river systems is currently sparse and represents an important knowledge gap in our understanding of the global carbon cycle. Here we examine variations in organic geochemical characteristics of suspended sediments from the Changjiang (Yangtze River) system collected between 1997 and 2010. Higher particulate organic carbon content (POC\%) values were observed in the middle reach, especially after 2003, and are attributed to the increase of in situ (aquatic) primary production associated with decreased total suspended matter concentrations. Corresponding C-14 values from depth profiles taken in 2009 and 2010 indicate spatial and temporal variations in POC sources within the basin. Two isotopic mass balance approaches were explored to quantitatively apportion different sources of Changjiang POM. Results indicate that contributions of biomass and pre-aged soil organic matter are dominant, regardless of hydrological conditions, with soil-derived organic carbon comprising 17-56\% of POC based on a Monte Carlo three-end-member mixing model. In contrast, binary mixing model calculations suggest that up to 80\% of POC (2009 samples only) derived from biospheric sources. The emplacement of the Three Gorges Dam and resulting trapping of sediment from the upper reach of the watershed resulted in a modification of POM C-14 ages in the reservoir. With the resulting decline in sediment load and increase in the proportion of modern POC in the lower reach, these changes in POM flux and composition of the Changjiang have significant implications for downstream carbon cycle processes.}, keywords = {Changjiang, organic carbon, radiocarbon, suspended particulate matter, Three Gorges Dam}, issn = {2169-8953}, doi = {10.1029/2017JG004285}, url = {http://doi.wiley.com/10.1029/2017JG004285http://onlinelibrary.wiley.com/wol1/doi/10.1029/2017JG004285/fullpdfhttps://api.wiley.com/onlinelibrary/tdm/v1/articles/10.1029\%2F2017JG004285}, author = {Wu, Ying and Eglinton, Timothy I. and Zhang, Jing and Montlu{\c c}on, Daniel B.} } @article {1280, title = {Arctic Deltaic Lake Sediments As Recorders of Fluvial Organic Matter Deposition}, volume = {4}, year = {2016}, month = {2016}, pages = {77}, abstract = {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.}, isbn = {2296-6463}, doi = {10.3389/feart.2016.00077}, url = {http://journal.frontiersin.org/article/10.3389/feart.2016.00077}, author = {Vonk, Jorien E. and Dickens, Angela F. and Giosan, Liviu and Hussain, Zainab A. and Kim, Bokyung and Zipper, Samuel C. and Holmes, Robert M. and Montlu{\c c}on, Daniel B. and Galy, Valier and Eglinton, Timothy I.} } @article { ISI:000368907500001, title = {Multimolecular tracers of terrestrial carbon transfer across the pan-Arctic: C-14 characteristics of sedimentary carbon components and their environmental controls}, journal = {GLOBAL BIOGEOCHEMICAL CYCLES}, volume = {29}, number = {{11}}, year = {2015}, month = {NOV}, pages = {1855-1873}, type = {Article}, abstract = {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 {\textquoteleft}{\textquoteleft}old{{\textquoteright}{\textquoteright}} 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.}, issn = {0886-6236}, doi = {10.1002/2015GB005204}, author = {Feng, Xiaojuan and Gustafsson, {\"O}rjan and Holmes, R. Max and Vonk, Jorien E. and van Dongen, Bart E. and Semiletov, Igor P. and Dudarev, Oleg V. and Yunker, Mark B. and Macdonald, Robie W. and Wacker, Lukas and Montlu{\c c}on, Daniel B. and Eglinton, Timothy I.} } @article {108, title = {14C and 13C characteristics of higher plant biomarkers in Washington margin surface sediments}, journal = {Geochimica et Cosmochimica Acta}, volume = {105}, year = {2013}, note = {id: 2267}, pages = {14-30}, abstract = {Plant wax lipids and lignin phenols are the two most common classes of molecular markers that are used to trace vascular plant-derived OM in the marine environment. However, their 13C and 14C compositions have not been directly compared, which can be used to constrain the flux and attenuation of terrestrial carbon in marine environment. In this study, we describe a revised method of isolating individual lignin phenols from complex sedimentary matrices for 14C analysis using high pressure liquid chromatography (HPLC) and compare this approach to a method utilizing preparative capillary gas chromatography (PCGC). We then examine in detail the 13C and 14C compositions of plant wax lipids and lignin phenols in sediments from the inner and mid shelf of the Washington margin that are influenced by discharge of the Columbia River. Plant wax lipids (including n-alkanes, n-alkanoic (fatty) acids, n-alkanols, and n-aldehydes) displayed significant variability in both δ13C (-28.3{\textperthousand} to -37.5{\textperthousand}) and Δ14C values (-204{\textperthousand} to +2{\textperthousand}), suggesting varied inputs and/or continental storage and transport histories. In contrast, lignin phenols exhibited similar δ13C values (between -30{\textperthousand} and -34{\textperthousand}) and a relatively narrow range of Δ14C values (-45{\textperthousand} to -150{\textperthousand}; HPLC-based measurement) that were similar to, or younger than, bulk OM (-195{\textperthousand} to -137{\textperthousand}). Moreover, lignin phenol 14C age correlated with the degradation characteristics of this terrestrial biopolymer in that vanillyl phenols were on average \~{}500 years older than syringyl and cinnamyl phenols that degrade faster in soils and sediments. The isotopic characteristics, abundance, and distribution of lignin phenols in sediments suggest that they serve as promising tracers of recently biosynthesized terrestrial OM during supply to, and dispersal within the marine environment. Lignin phenol 14C measurements may also provide useful constraints on the vascular plant end member in isotopic mixing models for carbon source apportionment, and for interpretation of sedimentary records of past vegetation dynamics.}, issn = {0016-7037}, doi = {10.1016/j.gca.2012.11.034}, url = {http://www.sciencedirect.com/science/article/pii/S0016703712006874}, author = {Feng, Xiaojuan and Benitez-Nelson, Bryan C. and Montlu{\c c}on, Daniel B. and Prahl, Fredrick G. and McNichol, Ann P. and Xu, Li and Repeta, Daniel J. and Eglinton, Timothy I.} } @article { ISI:000315194800002, title = {C-14 and C-13 characteristics of higher plant biomarkers in Washington margin surface sediments}, journal = {GEOCHIMICA ET COSMOCHIMICA ACTA}, volume = {105}, year = {2013}, month = {MAR 15}, pages = {14-30}, type = {Article}, abstract = {Plant wax lipids and lignin phenols are the two most common classes of molecular markers that are used to trace vascular plant-derived OM in the marine environment. However, their C-13 and C-14 compositions have not been directly compared, which can be used to constrain the flux and attenuation of terrestrial carbon in marine environment. In this study, we describe a revised method of isolating individual lignin phenols from complex sedimentary matrices for C-14 analysis using high pressure liquid chromatography (HPLC) and compare this approach to a method utilizing preparative capillary gas chromatography (PCGC). We then examine in detail the C-13 and C-14 compositions of plant wax lipids and lignin phenols in sediments from the inner and mid shelf of the Washington margin that are influenced by discharge of the Columbia River. Plant wax lipids (including n-alkanes, n-alkanoic (fatty) acids, n-alkanols, and n-aldehydes) displayed significant variability in both delta C-13 (-28.3 parts per thousand to -37.5 parts per thousand) and Delta C-14 values (-204 parts per thousand to +2 parts per thousand), suggesting varied inputs and/or continental storage and transport histories. In contrast, lignin phenols exhibited similar delta C-13 values (between -30 parts per thousand and -34 parts per thousand) and a relatively narrow range of Delta C-14 values (-45 parts per thousand to -150 parts per thousand; HPLC-based measurement) that were similar to, or younger than, bulk OM (-195 parts per thousand to -137 parts per thousand). Moreover, lignin phenol C-14 age correlated with the degradation characteristics of this terrestrial biopolymer in that vanillyl phenols were on average similar to 500 years older than syringyl and cinnamyl phenols that degrade faster in soils and sediments. The isotopic characteristics, abundance, and distribution of lignin phenols in sediments suggest that they serve as promising tracers of recently biosynthesized terrestrial OM during supply to, and dispersal within the marine environment. Lignin phenol C-14 measurements may also provide useful constraints on the vascular plant end member in isotopic mixing models for carbon source apportionment, and for interpretation of sedimentary records of past vegetation dynamics. (C) 2012 Elsevier Ltd. All rights reserved.}, issn = {0016-7037}, doi = {10.1016/j.gca.2012.11.034}, author = {Feng, Xiaojuan and Benitez-Nelson, Bryan C. and Montlu{\c c}on, Daniel B. and Prahl, Fredrick G. and McNichol, Ann P. and Xu, Li and Repeta, Daniel J. and Eglinton, Timothy I.} } @article {101, title = {Molecular and isotopic insights into particulate organic carbon sources and dynamics in Jordan Basin, Gulf of Maine}, journal = {Continental Shelf Research}, volume = {68}, year = {2013}, pages = {15-22}, abstract = {The carbon isotope and lipid biomarker composition of suspended particles and surface sediment was measured to examine the impact of sediment supply, redistribution and post-depositional alteration processes on organic matter cycling in the Gulf of Maine, a semi-enclosed shelf sea in the northwest Atlantic. A beam attenuation profile revealed a >50 m-thick benthic nepheloid layer (BNL) in the Jordan Basin at the time of sampling (April 2006). The relatively low radiocarbon content of suspended particulate organic carbon (POC) in the BNL indicates that up to 82\% of the POC in this layer was supplied from resuspension of sediment. The concentration of alkenones normalized to POC increased with increasing depth in the water column and was highest in the surface sediment. In contrast to these markers of surface ocean photoautotrophy, the vertical profiles for the concentration and composition of short-chain (C14{\textendash}C18) n-alkanoic acids provided evidence for enhanced heterotrophic processes near the top of the BNL. Suspended POC samples from two depths within the BNL exhibited marked differences in radiocarbon content and fatty acid composition, suggesting that biological activity and associated processes within the BNL are vertically heterogeneous.}, issn = {0278-4343}, doi = {10.1016/j.csr.2013.08.005}, url = {http://www.sciencedirect.com/science/article/pii/S0278434313002653}, author = {Hwang, Jeomshik and Montlu{\c c}on, Daniel B. and Pilskaln, Cynthia H. and Eglinton, Timothy I.} } @article { ISI:000267640400001, title = {High-sensitivity measurement of diverse vascular plant-derived biomarkers in high-altitude ice cores}, journal = {GEOPHYSICAL RESEARCH LETTERS}, volume = {36}, year = {2009}, month = {JUL 3}, type = {Article}, abstract = {Semi-volatile organic compounds derived from burned and fresh vascular plant sources and preserved in high-altitude ice fields were detected and identified through use of recently developed analytical tools. Specifically, stir bar sorptive extraction and thermal desorption coupled with gas chromatography/time-of-flight mass spectrometry allowed measurement of multiple biomarkers in small sample volumes (<= 30 ml). Among other compounds of interest, several diterpenoids, which suggest inputs from conifers and conifer burning, were identified in post-industrial era and older Holocene ice from the Sajama site in the Bolivian Andes, but not in a glacial period sample, consistent with aridity changes. Differences in biomarker assemblages between sites support the use of these compounds as regionally constrained recorders of vegetation and climate change. This study represents the first application of these analytical techniques to ice core research and the first indication that records of vegetation fires may be reconstructed from diterpenoids in ice. Citation: Makou, M. C., L. G. Thompson, D. B. Montlucon, and T. I. Eglinton (2009), High-sensitivity measurement of diverse vascular plant-derived biomarkers in high-altitude ice cores, Geophys. Res. Lett., 36, L13501, doi: 10.1029/2009GL037643.}, issn = {0094-8276}, doi = {10.1029/2009GL037643}, author = {Makou, Matthew C. and Thompson, Lonnie G. and Montlu{\c c}on, Daniel B. and Eglinton, Timothy I.} } @article {317, title = {A new look at old carbon in active margin sediments RID F-1809-2010}, journal = {Geology}, volume = {37}, year = {2009}, note = {id: 1987; PT: J; UT: WOS:000263842200012}, pages = {239-242}, abstract = {Recent studies suggest that as much as half of the organic carbon (OC) undergoing burial in the sediments of tectonically active continental margins may be the product of fossil shale weathering. These estimates rely on the assumption that vascular plant detritus spends little time sequestered in intermediate reservoirs such as soils, freshwater sediments, and river deltas, and thus only minimally contributes to the extraneously old (14)C ages of total organic matter often observed on adjacent shelves. Here we test this paradigm by measuring the (14)C and delta(13)C values of individual higher plant wax fatty acids as well as the d13C values of extractable alkanes isolated from the Eel River margin (California). The isotopic signatures of the long chain fatty acids indicate that vascular plant material has been sequestered for several thousand years before deposition. A coupled molecular isotope mass balance used to reassess the sedimentary carbon budget indicates that the fossil component is less abundant than previously estimated, with pre-aged terrestrial material instead composing a considerable proportion of all organic matter. If these findings are characteristic of other continental margins proximal to small mountainous rivers, then the importance of petrogenic OC burial in marine sediments may need to be reevaluated.}, issn = {0091-7613}, doi = {10.1130/G25351A.1}, author = {Drenzek, Nicholas J. and Hughen, Konrad A. and Montlu{\c c}on, Daniel B. and Southon, John R. and dos Santos, Guaciara M. and Druffel, Ellen R. M. and Giosan, Liviu and Eglinton, Timothy I.} } @article {1907, title = {Constraints on the origin of sedimentary organic carbon in the Beaufort Sea from coupled molecular 13C and 14C measurements}, journal = {Marine Chemistry}, volume = {103}, year = {2007}, note = {id: 1030}, month = {2007}, pages = {146-162}, author = {Drenzek, Nicholas J. and Montlu{\c c}on, Daniel B. and Yunker, Mark B. and Macdonald, Robie W. and Eglinton, Timothy I.} }