Shah
Sunita R.
Shah
Sunita R.
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ArticleProminent bacterial heterotrophy and sources of 13C-depleted fatty acids to the interior Canada Basin(Copernicus Publications on behalf of the European Geosciences Union, 2013-11-07) Shah, Sunita R. ; Griffith, David R. ; Galy, Valier ; McNichol, Ann P. ; Eglinton, Timothy I.In recent decades, the Canada Basin of the Arctic Ocean has experienced rapidly decreasing summer sea ice coverage and freshening of surface waters. It is unclear how these changes translate to deeper waters, particularly as our baseline understanding of organic carbon cycling in the deep basin is quite limited. In this study, we describe full-depth profiles of the abundance, distribution and carbon isotopic composition of fatty acids from suspended particulate matter at a seasonally ice-free station and a semi-permanently ice-covered station. Fatty acids, along with suspended particulate organic carbon (POC), are more concentrated and 13C-enriched under ice cover than in ice-free waters. But this influence, apparent at 50 m depth, does not propagate downward below 150 m depth, likely due to the weak biological pump in the central Canada Basin. Branched fatty acids have δ13C values that are similar to suspended POC at all depths and are more 13C-enriched than even-numbered saturated fatty acids at depths above 3000 m. These are likely to be produced in situ by heterotrophic bacteria incorporating organic carbon that is isotopically similar to total suspended POC. Below surface waters, there is also the suggestion of a source of saturated even-numbered fatty acids which could represent contributions from laterally advected organic carbon and/or from chemoautotrophic bacteria. At 3000 m depth and below, a greater relative abundance of long-chain (C20–24), branched and unsaturated fatty acids is consistent with a stronger influence of re-suspended sedimentary organic carbon. At these deep depths, two individual fatty acids (C12 and iso-C17) are significantly depleted in 13C, allowing for the possibility that methane oxidizing bacteria contribute fatty acids, either directly to suspended particulate matter or to shallow sediments that are subsequently mobilized and incorporated into suspended particulate matter within the deep basin.
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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 interlaboratory study of TEX86 and BIT analysis using high-performance liquid chromatography–mass spectrometry(American Geophysical Union, 2009-03-20) Schouten, Stefan ; Hopmans, Ellen C. ; van der Meer, Jaap ; Mets, Anchelique ; Bard, Edouard ; Bianchi, Thomas S. ; Diefendorf, Aaron ; Escala, Marina ; Freeman, Katharine H. ; Furukawa, Yoshihiro ; Huguet, Carme ; Ingalls, Anitra ; Menot, Guillemette ; Nederbragt, Alexandra J. ; Oba, Masahiro ; Pearson, Ann ; Pearson, Emma J. ; Rosell-Mele, Antoni ; Schaeffer, Philippe ; Shah, Sunita R. ; Shanahan, Timothy M. ; Smith, Richard W. ; Smittenberg, Rienk ; Talbot, Helen M. ; Uchida, Masao ; Van Mooy, Benjamin A. S. ; Yamamoto, Masanobu ; Zhang, Zhaohui ; Sinninghe Damste, Jaap S.Recently, two new proxies based on the distribution of glycerol dialkyl glycerol tetraethers (GDGTs) were proposed, i.e., the TEX86 proxy for sea surface temperature reconstructions and the BIT index for reconstructing soil organic matter input to the ocean. In this study, fifteen laboratories participated in a round robin study of two sediment extracts with a range of TEX86 and BIT values to test the analytical reproducibility and repeatability in analyzing these proxies. For TEX86 the repeatability, indicating intra-laboratory variation, was 0.028 and 0.017 for the two sediment extracts or ±1–2°C when translated to temperature. The reproducibility, indicating among-laboratory variation, of TEX86 measurements was substantially higher, i.e., 0.050 and 0.067 or ±3–4°C when translated to temperature. The latter values are higher than those obtained in round robin studies of Mg/Ca and U37 k′ paleothermometers, suggesting the need to primarily improve compatibility between labs. The repeatability of BIT measurements for the sediment with substantial amounts of soil organic matter input was relatively small, 0.029, but reproducibility was large, 0.410. This large variance could not be attributed to specific equipment used or a particular data treatment. We suggest that this may be caused by the large difference in the molecular weight in the GDGTs used in the BIT index, i.e., crenarchaeol versus the branched GDGTs. Potentially, this difference gives rise to variable responses in the different mass spectrometers used. Calibration using authentic standards is needed to establish compatibility between labs performing BIT measurements.
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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.
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ArticleCarbon isotopic evidence for microbial control of carbon supply to Orca Basin at the seawater–brine interface(Copernicus Publications on behalf of the European Geosciences Union, 2013-05-13) Shah, Sunita R. ; Joye, Samantha B. ; Brandes, Jay A. ; McNichol, Ann P.Orca Basin, an intraslope basin on the Texas-Louisiana continental slope, hosts a hypersaline, anoxic brine in its lowermost 200 m in which limited microbial activity has been reported. This brine contains a large reservoir of reduced and aged carbon, and appears to be stable at decadal time scales: concentrations and isotopic composition of dissolved inorganic (DIC) and organic carbon (DOC) are similar to measurements made in the 1970s. Both DIC and DOC are more "aged" within the brine pool than in overlying water, and the isotopic contrast between brine carbon and seawater carbon is much greater for DIC than DOC. While the stable carbon isotopic composition of brine DIC points towards a combination of methane and organic carbon remineralization as its source, radiocarbon and box model results point to the brine interface as the major source region for DIC, allowing for only limited oxidation of methane diffusing upwards from sediments. This conclusion is consistent with previous studies that identify the seawater–brine interface as the focus of microbial activity associated with Orca Basin brine. Isotopic similarities between DIC and DOC suggest a different relationship between these two carbon reservoirs than is typically observed in deep ocean basins. Radiocarbon values implicate the seawater–brine interface region as the likely source region for DOC to the brine as well as DIC.