3,018 research outputs found
Organic sulfur: a spatially variable and understudied component of marine organic matter
© The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Longnecker, K., Oswald, L., Soule, M. C. K., Cutter, G. A., & Kujawinski, E. B. Organic sulfur: a spatially variable and understudied component of marine organic matter. Limnology and Oceanography Letters, (2020), doi:10.1002/lol2.10149.Sulfur (S) is a major heteroatom in organic matter. This project evaluated spatial variability in the concentration and molecular‐level composition of organic sulfur along gradients of depth and latitude. We measured the concentration of total organic sulfur (TOS) directly from whole seawater. Our data reveal high variability in organic sulfur, relative to established variability in total organic carbon or nitrogen. The deep ocean contained significant amounts of organic sulfur, and the concentration of TOS in North Atlantic Deep Water (NADW) decreased with increasing age while total organic carbon remained stable. Analysis of dissolved organic matter extracts by ultrahigh resolution mass spectrometry revealed that 6% of elemental formulas contained sulfur. The sulfur‐containing compounds were structurally diverse, and showed higher numbers of sulfur‐containing elemental formulas as NADW moved southward. These measurements of organic sulfur in seawater provide the foundation needed to define the factors controlling organic sulfur in the global ocean.We thank Catherine Carmichael, Winifred Johnson, and Gretchen Swarr for assistance with sample collection and processing, and Joe Jennings for the analysis of inorganic nutrients. The help of the captain and crew of the R/V Knorr and the other cruise participants during the “DeepDOM” cruise is appreciated. Two anonymous reviewers and Patricia Soranno provided thorough comments that greatly improved the manuscript. The ultrahigh resolution mass spectrometry samples were analyzed at the WHOI FT‐MS Users' Facility that is funded by the National Science Foundation (grant OCE‐0619608) and the Gordon and Betty Moore Foundation (GMBF1214). This project was funded by NSF grants OCE‐1154320 (to EBK and KL), the W.M. Marquet Award (to KL), and OCE‐1435708 (to GAC). The authors declare no conflicts of interest
Multipole Expansion for Relativistic Coulomb Excitation
We derive a general expression for the multipole expansion of the
electro-magnetic interaction in relativistic heavy-ion collisions, which can be
employed in higher-order dynamical calculations of Coulomb excitation. The
interaction has diagonal as well as off-diagonal multipole components,
associated with the intrinsic and relative coordinates of projectile and
target. A simple truncation in the off-diagonal components gives excellent
results in first-order perturbation theory for distant collisions and for beam
energies up to 200 MeV/nucleon.Comment: 3 figures, Accepted for publication in Phys. Rev.
Dissolved organic matter produced by Thalassiosira pseudonana
Author Posting. © The Author(s), 2014. This is the author's version of the work. It is posted here by permission of Elsevier for personal use, not for redistribution. The definitive version was published in Marine Chemistry 168 (2015): 114-123, doi:10.1016/j.marchem.2014.11.003.Phytoplankton are significant producers of dissolved organic matter (DOM) in marine ecosystems but the identity and dynamics of this DOM remain poorly constrained. Knowledge on the identity and dynamics of DOM are crucial for understanding the molecular-level reactions at the base of the global carbon cycle. Here we apply emerging analytical and computational tools from metabolomics to investigate the composition of DOM produced by the centric diatom Thalassiosira pseudonana. We assessed both intracellular metabolites within T. pseudonana (the endo-metabolome) and extracellular metabolites released by T. pseudonana (the exo-metabolome). The intracellular metabolites had a more variable composition than the extracellular metabolites. We putatively identified novel compounds not previously associated with T. pseudonana as well as compounds that have previously been identified within T. pseudonana’s metabolic capacity (e.g. dimethylsulfoniopropionate and degradation products of chitin). The resulting information will provide the basis for future experiments to assess the impact of T. pseudonana on the composition of dissolved organic matter in marine environments.Instrumentation in the WHOI FT-MS facility was funded by the National Science Foundation MRI program (OCE-0619608) and by the Gordon and Betty T. Moore Foundation (Grant #1214). This work was supported by NSF grant OCE-0928424 to EBK
Extraction efficiency and quantification of dissolved metabolites in targeted marine metabolomics
© The Author(s), 2017. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Limnology and Oceanography: Methods 15 (2017): 417–428, doi:10.1002/lom3.10181.The field of metabolomics seeks to characterize the suite of small molecules that comprise the end-products of cellular regulation. Metabolomics has been used in biomedical applications as well as environmental studies that explore ecological and biogeochemical questions. We have developed a targeted metabolomics method using electrospray ionization–liquid chromatography tandem mass spectrometry to analyze metabolites dissolved in seawater. Preparation of samples from the marine environment presents challenges because dilute metabolites must be concentrated and desalted. We present the extraction efficiencies of 89 metabolites in our targeted method using solid phase extraction (SPE). In addition, we calculate the limits of detection and quantification for the metabolites in the method and compare the instrument response factors in five different matrices ranging from deionized water to spent medium from cultured marine microbes. High background organic matter content reduces the instrument response factor for only a small group of metabolites, yet enhances the extraction efficiency for other metabolites on the SPE cartridge used here, a modified styrene-divinylbenzene polymer called PPL. Aromatic or larger uncharged compounds, in particular, are reproducibly well retained on the PPL polymer. This method is suitable for the detection of dissolved metabolites in marine samples, with limits of detection ranging from < 1 pM to ∼ 2 nM dependent on the dual impacts of seawater matrix on extraction efficiency and on instrument response factors.Gordon and Betty Moore Foundation Grant Number: 3304;
National Science Foundation Grant Number: OCE-1154320;
Simons Foundation Internationa
Evidence for quorum sensing and differential metabolite production by a marine bacterium in response to DMSP
© The Author(s), 2016. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in The ISME Journal 10 (2016): 2304–2316, doi:10.1038/ismej.2016.6.Microbes, the foundation of the marine foodweb, do not function in isolation, but rather rely on molecular level interactions among species to thrive. Although certain types of interactions between autotrophic and heterotrophic microorganisms have been well documented, the role of specific organic molecules in regulating inter-species relationships and supporting growth are only beginning to be understood. Here, we examine one such interaction by characterizing the metabolic response of a heterotrophic marine bacterium, Ruegeria pomeroyi DSS-3, to growth on dimethylsulfoniopropionate (DMSP), an abundant organosulfur metabolite produced by phytoplankton. When cultivated on DMSP, R. pomeroyi synthesized a quorum-sensing molecule, N-(3-oxotetradecanoyl)-l-homoserine lactone, at significantly higher levels than during growth on propionate. Concomitant with the production of a quorum-sensing molecule, we observed differential production of intra- and extracellular metabolites including glutamine, vitamin B2 and biosynthetic intermediates of cyclic amino acids. Our metabolomics data indicate that R. pomeroyi changes regulation of its biochemical pathways in a manner that is adaptive for a cooperative lifestyle in the presence of DMSP, in anticipation of phytoplankton-derived nutrients and higher microbial density. This behavior is likely to occur on sinking marine particles, indicating that this response may impact the fate of organic matter.This research is funded in part by the Gordon and Betty Moore Foundation through Grant GBMF3304 as well as by the National Science Foundation (Grants OCE-0928424 and OCE-1154320)
Confirmation of a one-dimensional spin-1/2 Heisenberg system with ferromagnetic first-nearest-neighbor and antiferromagnetic second-nearest-neighbor interactions in RbCuMoO
We have investigated magnetic properties of RbCuMoO
powder. Temperature dependence of magnetic susceptibility and magnetic-field
dependence of magnetization have shown that this cuprate is a model compound of
a one-dimensional spin-1/2 Heisenberg system with ferromagnetic
first-nearest-neighbor (1NN) and antiferromagnetic second-nearest-neighbor
(2NN) competing interactions (competing system). Values of the 1NN and 2NN
interactions are estimated as K and K (). This value of suggests that the ground state is a
spin-singlet incommensurate state. In spite of relatively large and
, no magnetic phase transition appears down to 2 K, while an
antiferromagnetic transition occurs in other model compounds of the competing
system with ferromagnetic 1NN interaction. For that reason,
RbCuMoO is an ideal model compound to study properties of
the incommensurate ground state that are unconfirmed experimentally.Comment: 6 pages, 4 figure
Designing molecules to bypass the singlet-triplet bottleneck in the electroluminescence of organic light-emitting-diode materials
Electroluminescence in organic light emitting diode (OLED) materials occurs
via the recombination of excitonic electrons-hole pairs Only the singlet
excitons of commonly used OLED materials, e.g., Aluminum trihydroxyquinoline
(AlQ), decay radiatively, limiting the external quantum efficiency to a
maximum 25%. Thus 75% of the energy is lost due to the triplet bottleneck for
radiative recombination. We consider molecules derived from AlQ which
bypass the triplet bottleneck by designing structures which contain strong
spin-orbit coupling. As a first stage of this work, groundstate energies and
vertical excitation energies of Al-arsenoquinolines and Al-boroarsenoquinolines
are calculated. It is found that the substitution of N by As leads to very
favourable results, while the boron substitution leads to no advantage.Comment: 4 pages, 4 figue
Release of ecologically relevant metabolites by the cyanobacterium Synechococcus elongatus CCMP 1631
Author Posting. © The Author(s), 2015. This is the author's version of the work. It is posted here by permission of Society for Applied Microbiology for personal use, not for redistribution. The definitive version was published in Environmental Microbiology 17 (2015): 3949–3963, doi:10.1111/1462-2920.12899.Photoautotrophic plankton in the surface ocean release organic compounds that fuel secondary production by heterotrophic bacteria. Here we show that an abundant marine cyanobacterium, Synechococcus elongatus, contributes a variety of nitrogen-rich and sulfur-containing compounds to dissolved organic matter. A combination of targeted and untargeted metabolomics and genomic tools was used to characterize the intracellular and extracellular metabolites of S. elongatus. Aromatic compounds such as 4-hydroxybenzoic acid and phenylalanine, as well as nucleosides (e.g., thymidine, 5’-methylthioadenosine, xanthosine), the organosulfur compound 3-mercaptopropionate, and the plant auxin indole 3-acetic acid, were released by S. elongatus at multiple time points during its growth. Further, the amino acid kynurenine was found to accumulate in the media even though it was not present in the predicted metabolome of S. elongatus. This indicates that some metabolites, including those not predicted by an organism’s genome, are likely excreted into the environment as waste; however, these molecules may have broader ecological relevance if they are labile to nearby microbes. The compounds described herein provide excellent targets for quantitative analysis in field settings to assess the source and lability of dissolved organic matter in situ.This project was funded by the Gordon and Betty Moore Foundation through Grant #3304 to E. Kujawinski.2016-07-0
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