Beaupre
Steven R.
Beaupre
Steven R.
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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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PreprintRapid, high-resolution C-14 chronology of ooids( 2015-03) Beaupre, Steven R. ; Roberts, Mark L. ; Burton, Joshua R. ; Summons, Roger E.Ooids are small, spherical to ellipsoidal grains composed of concentric layers of CaCO3 that could potentially serve as biogeochemical records of the environments in which they grew. Such records, however, must be placed in the proper temporal context. Therefore, we developed a novel acidification system and employed an accelerator mass spectrometer (AMS) with a gas accepting ion source to obtain radiocarbon (14C) chronologies extending radially through ooids within one 8-hour workday. The method was applied to ooids from Highborne Cay, Bahamas and Shark Bay, Australia, yielding reproducible 14C chronologies, as well as constraints on the rates and durations of ooid growth and independent estimates of local 14C reservoir ages.
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PreprintOptimizing a microwave gas ion source for continuous-flow accelerator mass spectrometry( 2011-09) von Reden, Karl F. ; Roberts, Mark L. ; Burton, Joshua R. ; Beaupre, Steven R.A 2.45 GHz microwave ion source coupled with a magnesium charge exchange canal (CxC) has been successfully adapted to a large acceptance radiocarbon accelerator mass spectrometry system at the National Ocean Sciences AMS Facility (NOSAMS), Woods Hole Oceanographic Institution. CO2 samples from various preparation sources are injected into the source through a glass capillary at 370 µl/min. Routine system parameters are about 120 - 140 µA of negative 12C current after the CxC, leading to about 400 14C counts per second for a modern sample and implying a system efficiency of 0.2%. While these parameters already allow us to perform high quality AMS analyses on large samples, we are working on ways to improve the output of the ion source regarding emittance and efficiency. Modeling calculations suggest modifications in the extraction triode geometry, shape and size of the plasma chamber could improve emittance and hence ion transport efficiency. Results of experimental tests of these modifications are presented.
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PreprintCarbonate as sputter target material for rapid 14C AMS( 2012-04-17) Longworth, Brett E. ; Robinson, Laura F. ; Roberts, Mark L. ; Beaupre, Steven R. ; Burke, Andrea ; Jenkins, William J.This paper describes a technique for measuring the 14C content of carbonate samples by producing C-ions directly in the negative ion sputter source of an accelerator mass spectrometer (AMS) system. This direct analysis of carbonate material eliminates the time and expense of graphite preparation. Powdered carbonate is mixed with titanium powder, loaded into a target cartridge, and compressed. Beam currents for optimally sized carbonate targets (0.09-0.15 mg C) are typically 10-20% of those produced by optimally-sized graphite targets (0.5-1 mg C). Modern (>0.8 Fm) samples run by this method have standard deviations of 0.009 Fm or less, and near-modern samples run as unknowns agree with values from traditional hydrolysis/graphite to better than 2%. Targets with as little as 0.06 mg carbonate produce useable ion currents and results, albeit with increased error and larger blank. In its current state, direct sputtering is best applied to problems where a large number of analyses with lower precision are required. These applications could include age surveys of deep-sea corals for determination of historic population dynamics, to identify samples that would benefit from high precision analysis, and for growth rate studies of organisms forming carbonate skeletons.
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Working PaperUS SOLAS Science Report(Woods Hole Oceanographic Institution, 2021-12) Stanley, Rachel H. R. ; Bell, Tom G. ; Gao, Yuan ; Gaston, Cassandra J. ; Ho, David T. ; Kieber, David J. ; Mackey, Katherine R. M. ; Meskhidze, Nicholas ; Miller, William L. ; Potter, Henry ; Vlahos, Penny ; Yager, Patricia L. ; Alexander, Becky ; Beaupre, Steven R. ; Craig, Susanne E. ; Cutter, Gregory A. ; Emerson, Steven ; Frossard, Amanda A. ; Gasso, Santiago ; Haus, Brian K. ; Keene, William C. ; Landing, William M. ; Moore, Richard H. ; Ortiz-Suslow, David ; Palter, Jaime B. ; Paulot, Fabien ; Saltzman, Eric ; Thornton, Daniel ; Wozniak, Andrew S. ; Zamora, Lauren M. ; Benway, Heather M.The Surface Ocean – Lower Atmosphere Study (SOLAS) (http://www.solas-int.org/) is an international research initiative focused on understanding the key biogeochemical-physical interactions and feedbacks between the ocean and atmosphere that are critical elements of climate and global biogeochemical cycles. Following the release of the SOLAS Decadal Science Plan (2015-2025) (Brévière et al., 2016), the Ocean-Atmosphere Interaction Committee (OAIC) was formed as a subcommittee of the Ocean Carbon and Biogeochemistry (OCB) Scientific Steering Committee to coordinate US SOLAS efforts and activities, facilitate interactions among atmospheric and ocean scientists, and strengthen US contributions to international SOLAS. In October 2019, with support from OCB, the OAIC convened an open community workshop, Ocean-Atmosphere Interactions: Scoping directions for new research with the goal of fostering new collaborations and identifying knowledge gaps and high-priority science questions to formulate a US SOLAS Science Plan. Based on presentations and discussions at the workshop, the OAIC and workshop participants have developed this US SOLAS Science Plan. The first part of the workshop and this Science Plan were purposefully designed around the five themes of the SOLAS Decadal Science Plan (2015-2025) (Brévière et al., 2016) to provide a common set of research priorities and ensure a more cohesive US contribution to international SOLAS.
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PreprintA note on reporting of reservoir 14C disequilibria and age offsets( 2016-01) Soulet, Guillaume ; Skinner, Luke C. ; Beaupre, Steven R. ; Galy, ValierReservoir age offsets are widely used to correct marine and speleothem radiocarbon age measurements for various calibration purposes. They also serve as a powerful tracer for carbon cycle dynamics. However, a clear terminology regarding reservoir age offsets is lacking, sometimes leading to miscalculations. This note seeks to provide consistent conventions for reporting reservoir 14C disequilibria useful to a broad range of environmental sciences. This contribution introduces the F14R and δ14R metrics to express the relative 14C disequilibrium between two contemporaneous reservoirs and the R metric as the associated reservoir age offset.
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ArticlePhotochemical reactivity of ancient marine dissolved organic carbon(American Geophysical Union, 2012-09-20) Beaupre, Steven R. ; Druffel, Ellen R. M.Marine dissolved organic carbon (DOC) is the largest reservoir of reduced carbon in seawater and persists up to 4,000–6,000 conventional radiocarbon (14C) years on average. Photochemical degradation has been suggested as a geochemical sink for these long-lived molecules, yet there have been no studies relating photochemical lability to the 14C-ages of surface DOC. We observed apparent second order (2°) kinetics with respect to DOC and a strong trend from Δ14C-enriched to depleted values during exhaustive photomineralization of surface marine DOC with high energy UV light. Geochemically, these results suggest that surface DOC is an isotopically-heterogeneous mixture of molecules for which photochemical lability and 14C ages are correlated. Photochemical mineralization may therefore be an important control on the persistence of 14C-depleted DOC in the ocean.
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PreprintA gas-accepting ion source for Accelerator Mass Spectrometry : progress and applications( 2011-10-31) Roberts, Mark L. ; von Reden, Karl F. ; Burton, Joshua R. ; McIntyre, Cameron P. ; Beaupre, Steven R.The National Ocean Sciences Accelerator Mass Spectrometry (NOSAMS) facility at the Woods Hole Oceanographic Institution has developed an Accelerator Mass Spectrometry (AMS) system designed specifically for the analysis of 14C in a continuously flowing stream of carrier gas. A key part of the system is a gas-accepting microwave ion source. Recently, substantial progress has been made in the development of this source, having achieved ion currents rivaling that of a traditional graphite source (albeit at relatively low efficiency). Details and present performance of the gas source are given. Additionally, representative results obtained from coupling the source to both a gas chromatograph and gas bench are presented.
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ArticleRefractory dissolved organic matter has similar chemical characteristics but different radiocarbon signatures with depth in the marine water column(American Geophysical Union, 2023-04-04) White, Margot E. ; Nguyen, Tran B. ; Koester, Irina ; Lardie Gaylord, Mary C. ; Beman, J. Michael ; Smith, Kenneth L. ; McNichol, Ann P. ; Beaupré, Steven R. ; Aluwihare, Lihini I.The >5,000‐year radiocarbon age (14C‐age) of much of the 630 ± 30 Pg C oceanic dissolved organic carbon (DOC) reservoir remains an enigma in the marine carbon cycle. The fact that DOC is significantly older than dissolved inorganic carbon at every depth in the ocean forms the basis of our current framing of the marine DOC cycle, where some component persists over multiple cycles of ocean mixing. As a result, 14C‐depleted, aged DOC is hypothesized to be present as a uniform reservoir with a constant 14C signature and concentration throughout the water column. However, key requirements of this model, including direct observations of DOC with similar 14C signatures in the surface and deep ocean, have never been met. Despite decades of research, the distribution of Δ14C values in marine DOC remains a mystery. Here, we applied a thermal fractionation method to compare operationally defined refractory DOC (RDOC) from different depths in the North Pacific Ocean. We found that RDOC shares chemical characteristics (as recorded by OC bond strength) throughout the water column but does not share the same 14C signature. Our results support one part of the current paradigm—that RDOC is comprised of structurally related components throughout the ocean that form a “background” reservoir. However, in contrast to the current paradigm, our results are consistent with a vertical concentration gradient and a vertical and inter‐ocean Δ14C gradient for RDOC. The observed Δ14C gradient is compatible with the potential addition of pre‐aged DOC to the upper ocean.