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ArticleMarine organic carbon and radiocarbon – present and future challenges(Cambridge University Press, 2022-01-25) Druffel, Ellen R. M. ; Beaupre, Steven R. ; Grotheer, Hendrik ; Lewis, Christian B. ; McNichol, Ann P. ; Mollenhauer, Gesine ; Walker, Brett D.We discuss present and developing techniques for studying radiocarbon in marine organic carbon (C). Bulk DOC (dissolved organic C) Δ14C measurements reveal information about the cycling time and sources of DOC in the ocean, yet they are time consuming and need to be streamlined. To further elucidate the cycling of DOC, various fractions have been separated from bulk DOC, through solid phase extraction of DOC, and ultrafiltration of high and low molecular weight DOC. Research using 14C of DOC and particulate organic C separated into organic fractions revealed that the acid insoluble fraction is similar in 14C signature to that of the lipid fraction. Plans for utilizing this methodology are described. Studies using compound specific radiocarbon analyses to study the origin of biomarkers in the marine environment are reviewed and plans for the future are outlined. Development of ramped pyrolysis oxidation methods are discussed and scientific questions addressed. A modified elemental analysis (EA) combustion reactor is described that allows high particulate organic C sample throughput by direct coupling with the MIniCArbonDAtingSystem.
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ArticleRadiocarbon dating of alkenones from marine sediments : II. Assessment of carbon process blanks(Dept. of Geosciences, University of Arizona, 2005) Mollenhauer, Gesine ; Montlucon, Daniel B. ; Eglinton, Timothy I.We evaluate potential process blanks associated with radiocarbon measurement of microgram to milligram quantities of alkenones at the National Ocean Sciences Accelerator Mass Spectrometry (NOSAMS) facility. Two strategies to constrain the contribution of blanks to alkenone 14C dates were followed: 1) dating of samples of known age and 2) multiple measurements of identical samples. We show that the potential contamination associated with the procedure does not lead to a systematic bias of the results of alkenone dating to either younger or older ages. Our results indicate that alkenones record Δ14C of ambient DIC with an accuracy of approximately 10‰. A conservative estimate of measurement precision is 17‰ for modern samples. Alkenone 14C ages are expected to be reliable within 500 yr for samples younger than 10,500 14C yr.
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PreprintRapid lateral particle transport in the Argentine Basin : molecular C-14 and Th-230(xs) evidence( 2006-05-06) Mollenhauer, Gesine ; McManus, Jerry F. ; Benthien, Albert ; Muller, Peter J. ; Eglinton, Timothy I.Recent studies have revealed that lateral transport and focusing of particles strongly influences the depositional patterns of organic matter in marine sediments. Transport can occur in the water column prior to initial deposition or following sediment re-suspension. In both cases, fine-grained particles and organic-rich aggregates are more susceptible to lateral transport than coarse-grained particles (e.g. foraminiferal tests) because of the slower sinking velocities of the former. This may lead to spatial and, in the case of redistribution of resuspended sediments, temporal decoupling of organic matter from coarser sediment constituents. Prior studies from the Argentine Basin have yielded evidence that suspended particles are displaced significant distances (100 - 1000 km) northward and downslope by strong surface and/or bottom currents. These transport processes result in anomalously cold alkenone-derived sea surface temperature (SST) estimates (up to 6°C colder than measured SST) and in the presence of frustules of Antarctic diatom species in surface sediments fromthis area. Here we examine advective transport processes through combined measurements of compound-specific radiocarbon ages of marine phytoplankton derived biomarkers (alkenones) from core-tops and excess 230Th (230Thxs)-derived focusing factors for late Holocene sediments from the Argentine Basin. On the continental slope, we observe 230Thxs-based focusing factors of 1.4 to 3.2 at sites where alkenone-based SST estimates were 4–6°C colder than measured values. In contrast, alkenone radiocarbon data suggest coeval deposition of marine biomarkers and planktic foraminifera, as alkenones in core-tops were younger than, or similar in age to, foraminifera. We therefore infer that the transport processes leading to the lateral displacement of these sediment components are rapid, and hence probably occur in the upper water column (<1500 m).
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PreprintTimescales of lateral sediment transport in the Panama Basin as revealed by radiocarbon ages of alkenones, total organic carbon and foraminifera( 2009-12) Kusch, Stephanie ; Eglinton, Timothy I. ; Mix, Alan C. ; Mollenhauer, GesinePaired radiocarbon measurements on haptophyte biomarkers (alkenones) and on cooccurring tests of planktic foraminifera (Neogloboquadrina dutertrei and Globogerinoides sacculifer) from late glacial to Holocene sediments at core locations ME0005-24JC, Y69- 71P, and MC16 from the south-western and central Panama Basin indicate no significant addition of pre-aged alkenones by lateral advection. The strong temporal correspondence between alkenones, foraminifera and total organic carbon (TOC) also implies negligible contributions of aged terrigenous material. Considering controversial evidence for sediment redistribution in previous studies of these sites, our data imply that the laterally supplied material cannot stem from remobilization of substantially aged sediments. Transport, if any, requires syn-depositional nepheloid layer transport and redistribution of low-density or fine-grained components within decades of particle formation. Such rapid and local transport minimizes the potential for temporal decoupling of proxies residing in different grain size fractions and thus facilitates comparison of various proxies for paleoceanographic reconstructions in this study area. Anomalously old foraminiferal tests from a glacial depth interval of core Y69-71P may result from episodic spillover of fast bottom currents across the Carnegie Ridge transporting foraminiferal sands towards the north.
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PreprintA radiocarbon-based assessment of the preservation characteristics of crenarchaeol and alkenones from continental margin sediments( 2008-01-22) Mollenhauer, Gesine ; Eglinton, Timothy I. ; Hopmans, Ellen C. ; Sinninghe Damste, Jaap S.Crenarchaeotal glycerol dibiphytanyl glycerol tetraether (GDGT) lipids and alkenones are two types of biomarkers derived from planktonic marine micro-organisms which are used for reconstruction of sea-surface temperatures. We determined the radiocarbon contents of the archaeal GDGT crenarchaeol and of alkenones isolated from continental margin sediments. Systematic differences were found between the two biomarkers, with higher radiocarbon contents in crenarchaeol than in the phytoplankton-derived alkenones. These differences can be explained by variable contributions of pre-aged, laterally advected material to the core sites. Crenarchaeol appears to be more efficiently degraded during transport in oxygen-replete environments than alkenones. Whether this reflects the influence of chemical structure or mode of protection (e.g., particle association) is not yet known.
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ArticleOn the sedimentological origin of down-core variations of bulk sedimentary nitrogen isotope ratios(American Geophysical Union, 2005-05-27) Kienast, Markus ; Higginson, M. J. ; Mollenhauer, Gesine ; Eglinton, Timothy I. ; Chen, Min-Te ; Calvert, Stephen E.The bulk sedimentary nitrogen isotopic composition of two cores from nearby sites on the northern slope of the South China Sea (Site 17940 and Ocean Drilling Program (ODP) Site 1144) differs by up to >2‰ during the last glacial period. Given their close proximity, both core sites are located in the same biogeographic zone and nutrient regime, and it is thus unlikely that this offset is due to a true gradient in surface ocean conditions. In an attempt to resolve this offset, we have investigated the possible effects of two sedimentological parameters that can affect bulk sedimentary δ15N, namely, the variable contribution of inorganic N to bulk N in the sediment and the grain-size dependence of bulk δ15N. We find that neither effect, singly or in combination, is sufficient to explain the significant δ15N offset between the two down-core records. By elimination the most likely explanation for the observed discrepancy is a different origin of both the organic and inorganic nitrogen at each site. This study adds to the growing body of evidence highlighting the complex nature and origin of the sedimentary components in sediment drifts, such as ODP Site 1144.
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ArticleParticulate organic carbon deconstructed: molecular and chemical composition of particulate organic carbon in the ocean(Frontiers Media, 2020-06-26) Kharbush, Jenan J. ; Close, Hilary G. ; Van Mooy, Benjamin A. S. ; Arnosti, Carol ; Smittenberg, Rienk H. ; Le Moigne, Frederic A. C. ; Mollenhauer, Gesine ; Scholz-Böttcher, Barbara ; Obreht, Igor ; Koch, Boris P. ; Becker, Kevin W. ; Iversen, Morten H. ; Mohr, WiebkeThe dynamics of the particulate organic carbon (POC) pool in the ocean are central to the marine carbon cycle. POC is the link between surface primary production, the deep ocean, and sediments. The rate at which POC is degraded in the dark ocean can impact atmospheric CO2 concentration. Therefore, a central focus of marine organic geochemistry studies is to improve our understanding of POC distribution, composition, and cycling. The last few decades have seen improvements in analytical techniques that have greatly expanded what we can measure, both in terms of organic compound structural diversity and isotopic composition, and complementary molecular omics studies. Here we provide a brief overview of the autochthonous, allochthonous, and anthropogenic components comprising POC in the ocean. In addition, we highlight key needs for future research that will enable us to more effectively connect diverse data sources and link the identity and structural diversity of POC to its sources and transformation processes.
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ArticleSelective preservation of organic matter in marine environments; processes and impact on the sedimentary record(Copernicus Publications on behalf of the European Geosciences Union, 2010-02-05) Zonneveld, K. A. F. ; Versteegh, G. J. M. ; Kasten, S. ; Eglinton, Timothy I. ; Emeis, Kay-Christian ; Huguet, Carme ; Koch, Boris P. ; de Lange, Gert J. ; de Leeuw, J. W. ; Middelburg, Jack J. ; Mollenhauer, Gesine ; Prahl, Fredrick G. ; Rethemeyer, J. ; Wakeham, Stuart G.The present paper is the result of a workshop sponsored by the DFG Research Center/Cluster of Excellence MARUM "The Ocean in the Earth System", the International Graduate College EUROPROX, and the Alfred Wegener Institute for Polar and Marine Research. The workshop brought together specialists on organic matter degradation and on proxy-based environmental reconstruction. The paper deals with the main theme of the workshop, understanding the impact of selective degradation/preservation of organic matter (OM) in marine sediments on the interpretation of the fossil record. Special attention is paid to (A) the influence of the molecular composition of OM in relation to the biological and physical depositional environment, including new methods for determining complex organic biomolecules, (B) the impact of selective OM preservation on the interpretation of proxies for marine palaeoceanographic and palaeoclimatic reconstruction, and (C) past marine productivity and selective preservation in sediments. It appears that most of the factors influencing OM preservation have been identified, but many of the mechanisms by which they operate are partly, or even fragmentarily, understood. Some factors have not even been taken carefully into consideration. This incomplete understanding of OM breakdown hampers proper assessment of the present and past carbon cycle as well as the interpretation of OM based proxies and proxies affected by OM breakdown. To arrive at better proxy-based reconstructions "deformation functions" are needed, taking into account the transport and diagenesis-related molecular and atomic modifications following proxy formation. Some emerging proxies for OM degradation may shed light on such deformation functions. The use of palynomorph concentrations and selective changes in assemblage composition as models for production and preservation of OM may correct for bias due to selective degradation. Such quantitative assessment of OM degradation may lead to more accurate reconstruction of past productivity and bottom water oxygenation. Given the cost and effort associated with programs to recover sediment cores for paleoclimatological studies, as well as with generating proxy records, it would seem wise to develop a detailed sedimentological and diagenetic context for interpretation of these records. With respect to the latter, parallel acquisition of data that inform on the fidelity of the proxy signatures and reveal potential diagenetic biases would be of clear value.
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PreprintOrigins of archaeal tetraether lipids in sediments : insights from radiocarbon analysis( 2008-06-20) Shah, Sunita R. ; Mollenhauer, Gesine ; Ohkouchi, Naohiko ; Eglinton, Timothy I. ; Pearson, AnnUnderstanding the supply and preservation of glycerol dibiphytanyl glycerol tetraethers (GDGTs) in marine sediments helps inform their use in paleoceanography. Compound-specific radiocarbon measurements of sedimentary alkenones from multiple environments have been used to gain insight into processes that affect paleo-temperature reconstructions. Similar analyses are warranted to investigate how analogous processes affecting GDGTs impact TEX86 paleotemperatures. Here we present radiocarbon measurements on individual GDGTs from Bermuda Rise and Santa Monica Basin sediments and discuss the results in the context of previous studies of co-depositional alkenones and foraminifera. The 149 C contents of GDGTs and planktonic foraminifera in Bermuda Rise are very similar, suggesting a local source; and TEX86- derived temperatures agree more closely with foraminiferal temperatures than do temperatures. In contrast, GDGTs in Santa Monica Basin are depleted in 1412 C relative to both alkenones and foraminifera, and TEX86 temperatures agree poorly with known surface water values. We propose three possible factors that could explain these results: (i) GDGTs may be labile relative to alkenones during advective transport through oxic waters; (ii) archaeal production deep in the water column may contribute 1416 C-depleted GDGTs to sediments; and (iii) some GDGTs also may derive from sedimentary archaeal communities. Each of these three processes is likely to occur with varying relative importance depending on geographic location. The latter two may help to explain why TEX86 temperature reconstructions from Santa Monica Basin do not appear to reflect actual sea surface temperatures. Terrigenous GDGTs are unlikely to be major contributors to Bermuda Rise or Santa Monica Basin sediments, based on values of the BIT index. The results also indicate that the crenarchaeol regioisomer is governed by processes different from other GDGTs. Individual measurements of the crenarchaeol regioisomer are significantly depleted in 1424 C relative to co-occurring GDGTs, indicating an alternative origin for this compound that presently remains unknown. Re-examination of the contribution of crenarchaeol regioisomer to the TEX86 index shows that it is a significant influence on the sensitivity of temperature reconstructions.
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ArticleAn evaluation of 14C age relationships between co-occurring foraminifera, alkenones, and total organic carbon in continental margin sediments(American Geophysical Union, 2005-01-25) Mollenhauer, Gesine ; Kienast, Markus ; Lamy, Frank ; Meggers, Helge ; Schneider, Ralph R. ; Hayes, John M. ; Eglinton, Timothy I.Radiocarbon age relationships between co-occurring planktic foraminifera, alkenones and total organic carbon in sediments from the continental margins of Southern Chile, Northwest Africa and the South China Sea were compared with published results from the Namibian margin. Age relationships between the sediment components are site-specific and relatively constant over time. Similar to the Namibian slope, where alkenones have been reported to be 1000 to 4500 years older than co-occurring foraminifera, alkenones were significantly (~1000 yrs) older than co-occurring foraminifera in the Chilean margin sediments. In contrast, alkenones and foraminifera were of similar age (within 2σ error or better) in the NW African and South China Sea sediments. Total-organic-matter and alkenone ages were similar off Namibia (age difference TOC-alkenones: 200-700 years), Chile (100-450 years), and NW Africa (360-770 years), suggesting minor contributions of pre-aged terrigenous material. In the South China Sea total organic carbon is significantly (2000-3000 yrs) older due to greater inputs of pre-aged terrigenous material. Age offsets between alkenones and planktic foraminifera are attributed to lateral advection of organic matter. Physical characteristics of the depositional setting, such as sea-floor morphology, shelf width, and sediment composition, may control the age of co-occurring 2 sediment components. In particular, offsets between alkenones and foraminifera appear to be greatest in deposition centers in morphologic depressions. Aging of organic matter is promoted by transport. Age offsets are correlated with organic richness, suggesting that formation of organic aggregate is a key process.
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ArticleConsistently dated Atlantic sediment cores over the last 40 thousand years(Nature Research, 2019-09-02) Waelbroeck, Claire ; Lougheed, Bryan C. ; Vazquez Riveiros, Natalia ; Missiaen, Lise ; Pedro, Joel ; Dokken, Trond ; Hajdas, Irka ; Wacker, Lukas ; Abbott, Peter ; Dumoulin, Jean-Pascal ; Thil, Francois ; Eynaud, Frederique ; Rossignol, Linda ; Fersi, Wiem ; Albuquerque, Ana Luiza ; Arz, Helge W. ; Austin, William E. N. ; Came, Rosemarie E. ; Carlson, Anders E. ; Collins, James A. ; Dennielou, Bernard ; Desprat, Stéphanie ; Dickson, Alex ; Elliot, Mary ; Farmer, Christa ; Giraudeau, Jacques ; Gottschalk, Julia ; Henderiks, Jorijntje ; Hughen, Konrad A. ; Jung, Simon ; Knutz, Paul ; Lebreiro, Susana ; Lund, David C. ; Lynch-Stieglitz, Jean ; Malaizé, Bruno ; Marchitto, Thomas M. ; Martínez-Méndez, Gema ; Mollenhauer, Gesine ; Naughton, Filipa ; Nave, Silvia ; Nürnberg, Dirk ; Oppo, Delia W. ; Peck, Vicky L. ; Peeters, Frank J. C. ; Penaud, Aurélie ; Portilho-Ramos, Rodrigo da Costa ; Repschläger, Janne ; Roberts, Jenny ; Ruhlemann, Carsten ; Salgueiro, Emilia ; Sanchez Goni, Maria Fernanda ; Schönfeld, Joachim ; Scussolini, Paolo ; Skinner, Luke C. ; Skonieczny, Charlotte ; Thornalley, David J. R. ; Toucanne, Samuel ; Van Rooij, David ; Vidal, Laurence ; Voelker, Antje H. L. ; Wary, Mélanie ; Weldeab, Syee ; Ziegler, MartinRapid changes in ocean circulation and climate have been observed in marine-sediment and ice cores over the last glacial period and deglaciation, highlighting the non-linear character of the climate system and underlining the possibility of rapid climate shifts in response to anthropogenic greenhouse gas forcing. To date, these rapid changes in climate and ocean circulation are still not fully explained. One obstacle hindering progress in our understanding of the interactions between past ocean circulation and climate changes is the difficulty of accurately dating marine cores. Here, we present a set of 92 marine sediment cores from the Atlantic Ocean for which we have established age-depth models that are consistent with the Greenland GICC05 ice core chronology, and computed the associated dating uncertainties, using a new deposition modeling technique. This is the first set of consistently dated marine sediment cores enabling paleoclimate scientists to evaluate leads/lags between circulation and climate changes over vast regions of the Atlantic Ocean. Moreover, this data set is of direct use in paleoclimate modeling studies.
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ArticleAging of marine organic matter during cross-shelf lateral transport in the Benguela upwelling system revealed by compound-specific radiocarbon dating(American Geophysical Union, 2007-09-18) Mollenhauer, Gesine ; Inthorn, Maik ; Vogt, Thomas ; Zabel, Matthias ; Sinninghe Damste, Jaap S. ; Eglinton, Timothy I.Organic matter accumulation and burial on the Namibian shelf and upper slope are spatially heterogeneous and strongly controlled by lateral transport in subsurface nepheloid layers. Much of the material deposited in depo-centers on the slope ultimately derives from the shelf. Supply of organic matter from the shelf involves selective transport of organic matter. We studied these selective transport processes by analyzing the radiocarbon content of co-occurring sediment fractions. Here we present radiocarbon data for total organic carbon as well as three tracers of surface ocean productivity (phytoplankton-derived alkenones, membrane lipids of pelagic crenarchaeota (crenarchaeol), and calcareous microfossils of planktic foraminifera) in core-top and near-surface sediment samples. The samples were collected on the Namibian margin along a shelf-slope transect (85 to 1040 m) at 24°S and from the upper slope depo-center at 25.5°S. In core-top sediments, alkenone ages gradually increased from modern to 3490 radiocarbon years with distance from shore and with water depth. Crenarchaeol, while younger than alkenones, also increased in age with distance offshore. It was concluded that the observed ages were a consequence of cross-shelf transport and associated aging of organic matter. Radiocarbon ages of preserved lipid biomarkers in sediments thus at least partially depend on the relative amount of laterally supplied, pre-aged material present in a sample, highlighting the importance of nepheloid transport for the sedimentation of organic matter over the Namibian margin.
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ArticleAn interlaboratory study of TEX86 and BIT analysis of sediments, extracts, and standard mixtures(John Wiley & Sons, 2013-12-20) Schouten, Stefan ; Hopmans, Ellen C. ; Rosell-Mele, Antoni ; Pearson, Ann ; Adam, Pierre ; Bauersachs, Thorsten ; Bard, Edouard ; Bernasconi, Stefano M. ; Bianchi, Thomas S. ; Brocks, Jochen J. ; Carlson, Laura Truxal ; Castaneda, Isla S. ; Derenne, Sylvie ; Selver, Ayca Dogrul ; Dutta, Koushik ; Eglinton, Timothy I. ; Fosse, Celine ; Galy, Valier ; Grice, Kliti ; Hinrichs, Kai-Uwe ; Huang, Yongsong ; Huguet, Arnaud ; Huguet, Carme ; Hurley, Sarah ; Ingalls, Anitra ; Jia, Guodong ; Keely, Brendan ; Knappy, Chris ; Kondo, Miyuki ; Krishnan, Srinath ; Lincoln, Sara ; Lipp, Julius S. ; Mangelsdorf, Kai ; Martínez-Garcia, Alfredo ; Menot, Guillemette ; Mets, Anchelique ; Mollenhauer, Gesine ; Ohkouchi, Naohiko ; Ossebaar, Jort ; Pagani, Mark ; Pancost, Richard D. ; Pearson, Emma J. ; Peterse, Francien ; Reichart, Gert-Jan ; Schaeffer, Philippe ; Schmitt, Gaby ; Schwark, Lorenz ; Shah, Sunita R. ; Smith, Richard W. ; Smittenberg, Rienk H. ; Summons, Roger E. ; Takano, Yoshinori ; Talbot, Helen M. ; Taylor, Kyle W. R. ; Tarozo, Rafael ; Uchida, Masao ; van Dongen, Bart E. ; Van Mooy, Benjamin A. S. ; Wang, Jinxiang ; Warren, Courtney ; Weijers, Johan W. H. ; Werne, Josef P. ; Woltering, Martijn ; Xie, Shucheng ; Yamamoto, Masanobu ; Yang, Huan ; Zhang, Chuanlun L. ; Zhang, Yige ; Zhao, Meixun ; Sinninghe Damste, Jaap S.Two commonly used proxies based on the distribution of glycerol dialkyl glycerol tetraethers (GDGTs) are the TEX86 (TetraEther indeX of 86 carbon atoms) paleothermometer for sea surface temperature reconstructions and the BIT (Branched Isoprenoid Tetraether) index for reconstructing soil organic matter input to the ocean. An initial round-robin study of two sediment extracts, in which 15 laboratories participated, showed relatively consistent TEX86 values (reproducibility ±3–4°C when translated to temperature) but a large spread in BIT measurements (reproducibility ±0.41 on a scale of 0–1). Here we report results of a second round-robin study with 35 laboratories in which three sediments, one sediment extract, and two mixtures of pure, isolated GDGTs were analyzed. The results for TEX86 and BIT index showed improvement compared to the previous round-robin study. The reproducibility, indicating interlaboratory variation, of TEX86 values ranged from 1.3 to 3.0°C when translated to temperature. These results are similar to those of other temperature proxies used in paleoceanography. Comparison of the results obtained from one of the three sediments showed that TEX86 and BIT indices are not significantly affected by interlaboratory differences in sediment extraction techniques. BIT values of the sediments and extracts were at the extremes of the index with values close to 0 or 1, and showed good reproducibility (ranging from 0.013 to 0.042). However, the measured BIT values for the two GDGT mixtures, with known molar ratios of crenarchaeol and branched GDGTs, had intermediate BIT values and showed poor reproducibility and a large overestimation of the “true” (i.e., molar-based) BIT index. The latter is likely due to, among other factors, the higher mass spectrometric response of branched GDGTs compared to crenarchaeol, which also varies among mass spectrometers. Correction for this different mass spectrometric response showed a considerable improvement in the reproducibility of BIT index measurements among laboratories, as well as a substantially improved estimation of molar-based BIT values. This suggests that standard mixtures should be used in order to obtain consistent, and molar-based, BIT values.