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  • 2015-2019  (4)
  • 2017  (4)
  • 1
    Publication Date: 2018-01-10
    Description: © The Author(s), 2017. This is the author's version of the work. It is posted here under a nonexclusive, irrevocable, paid-up, worldwide license granted to WHOI. It is made available for personal use, not for redistribution. The definitive version was published in Deep Sea Research Part I: Oceanographic Research Papers 125 (2017): 106-128, doi:10.1016/j.dsr.2017.05.003.
    Description: The high particle reactivity of thorium has resulted in its widespread use in tracing processes impacting marine particles and their chemical constituents. The use of thorium isotopes as tracers of particle dynamics, however, largely relies on our understanding of how the element scavenges onto particles. Here, we estimate apparent rate constants of Th adsorption (k1), Th desorption (k−1), bulk particle degradation (β-1), and bulk particle sinking speed (w) along the water column at 11 open-ocean stations occupied during the GEOTRACES North Atlantic Section (GA03). First, we provide evidence that the budgets of Th isotopes and particles at these stations appear to be generally dominated by radioactive production and decay sorption reactions, particle degradation, and particle sinking. Rate parameters are then estimated by fitting a Th and particle cycling model to data of dissolved and particulate 228,230,234Th, 228Ra, particle concentrations, and 234,238U estimates based on salinity, using a nonlinear programming technique. We find that the adsorption rate constant (k1) generally decreases with depth across the section: broadly, the time scale 1/k1 averages 1.0 yr in the upper 1000 m and (1.4–1.5) yr below. A positive relationship between k1 and particle concentration (P) is found, i.e., , k1 ∝ Pb where b ≥ 1, consistent with the notion that k1 increases with the number of surface sites available for adsorption. The rate constant ratio, K = k1/(k-1 + β-1), which measures the collective influence of rate parameters on Th scavenging, averages 0.2 for most stations and most depths. We clarify the conditions under which K/P is equivalent to the distribution coefficient, KD, test that the conditions are met at the stations, and find that decreases with P, in line with a particle concentration effect (dKD/dP 〈 0). In contrast to the influence of colloids as envisioned by the Brownian pumping hypothesis, we provide evidence that the particle concentration effect arises from the joint effect of P on the rate constants for thorium attachment to, and detachment from, particles.
    Description: We acknowledge the U.S. National Science Foundation for providing funding for this study (grant OCE-1232578) and for U.S. GEOTRACES North Atlantic section ship time, sampling, and data analysis. The U.S. NSF also supported the generation of 230Th data (OCE-0927064 to LDEO, OCE-O092860 to WHOI, and OCE-0927754 to UMN) and 228,234Th data (OCE-0925158 to WHOI).
    Keywords: GEOTRACES ; Thorium ; Particle Concentration Effect ; Single-particle class model ; Inverse method
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 2
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    Copernicus Publications on behalf of the European Geosciences Union
    Publication Date: 2017-11-13
    Description: © The Author(s), 2017. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Cryosphere 11 (2017): 2439-2462, doi:10.5194/tc-11-2439-2017.
    Description: Methanesulfonic acid (MSA; CH3SO3H) in polar ice is a unique proxy of marine primary productivity, synoptic atmospheric transport, and regional sea-ice behavior. However, MSA can be mobile within the firn and ice matrix, a post-depositional process that is well known but poorly understood and documented, leading to uncertainties in the integrity of the MSA paleoclimatic signal. Here, we use a compilation of 22 ice core MSA records from Greenland and Antarctica and a model of soluble impurity transport in order to comprehensively investigate the vertical migration of MSA from summer layers, where MSA is originally deposited, to adjacent winter layers in polar ice. We find that the shallowest depth of MSA migration in our compilation varies over a wide range (∼ 2 to 400 m) and is positively correlated with snow accumulation rate and negatively correlated with ice concentration of Na+ (typically the most abundant marine cation). Although the considered soluble impurity transport model provides a useful mechanistic framework for studying MSA migration, it remains limited by inadequate constraints on key physico-chemical parameters – most notably, the diffusion coefficient of MSA in cold ice (DMS). We derive a simplified version of the model, which includes DMS as the sole parameter, in order to illuminate aspects of the migration process. Using this model, we show that the progressive phase alignment of MSA and Na+ concentration peaks observed along a high-resolution West Antarctic core is most consistent with 10−12 m2 s−1 〈 DMS 〈 10−11 m2 s−1, which is 1 order of magnitude greater than the DMS values previously estimated from laboratory studies. More generally, our data synthesis and model results suggest that (i) MSA migration may be fairly ubiquitous, particularly at coastal and (or) high-accumulation regions across Greenland and Antarctica; and (ii) can significantly change annual and multiyear MSA concentration averages. Thus, in most cases, caution should be exercised when interpreting polar ice core MSA records, although records that have undergone severe migration could still be useful for inferring decadal and lower-frequency climate variability.
    Description: Matthew Osman acknowledges government support awarded by DoD, Air Force Office of Scientific Research, National Defense Science and Engineering Graduate (NDSEG) Fellowship, 32 CFR 168a. This work was supported by the US NSF (ANT-0632031 and PLR-1205196 to Sarah B. Das, and NSF-MRI-1126217 to Matthew J. Evans) and a Woods Hole Oceanographic Institution Interdisciplinary Research award to Sarah B. Das and Olivier Marchal.
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 3
    Publication Date: 2017-05-19
    Description: Methanesulfonic acid (MSA; CH3SO3H) in polar ice is a unique proxy of marine primary productivity, synoptic atmospheric transport, and regional sea ice behavior. However, MSA can be mobile within the firn and ice matrix, a post-depositional process that is well known but poorly understood and documented, leading to uncertainties in the integrity of the MSA paleoclimatic signal. Here, we use a compilation of 22 ice core MSA records from Greenland and Antarctica and a model of soluble impurity transport in order to comprehensively investigate the vertical migration of MSA from summer layers, where MSA is originally deposited, to adjacent winter layers in polar ice. The shallowest depths of MSA migration reported in our compilation vary over a wide range (~ 2 m to 400 m), and our analysis suggests that these depths are positively correlated with snow accumulation rate and negatively correlated with ice concentration of Na+ (typically the most abundant cationic sea salt). Although the considered soluble impurity transport model provides a useful mechanistic framework for studying MSA migration, it remains limited by inadequate constraints on key physicochemical parameters, most notably, the diffusion coefficient of MSA in cold ice (DMS). We derive a simplified version of the model, which includes DMS as the sole parameter, in order to illuminate aspects of the migration process. Using this model, we show that the progressive phase alignment of MSA and Na+ concentration peaks observed along a high-resolution West Antarctic core is most consistent with 10–12 m2 s-1 
    Print ISSN: 1994-0432
    Electronic ISSN: 1994-0440
    Topics: Geography , Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 4
    Publication Date: 2017-11-03
    Description: Methanesulfonic acid (MSA; CH3SO3H) in polar ice is a unique proxy of marine primary productivity, synoptic atmospheric transport, and regional sea-ice behavior. However, MSA can be mobile within the firn and ice matrix, a post-depositional process that is well known but poorly understood and documented, leading to uncertainties in the integrity of the MSA paleoclimatic signal. Here, we use a compilation of 22 ice core MSA records from Greenland and Antarctica and a model of soluble impurity transport in order to comprehensively investigate the vertical migration of MSA from summer layers, where MSA is originally deposited, to adjacent winter layers in polar ice. We find that the shallowest depth of MSA migration in our compilation varies over a wide range (∼2 to 400m) and is positively correlated with snow accumulation rate and negatively correlated with ice concentration of Na+ (typically the most abundant marine cation). Although the considered soluble impurity transport model provides a useful mechanistic framework for studying MSA migration, it remains limited by inadequate constraints on key physico-chemical parameters – most notably, the diffusion coefficient of MSA in cold ice (DMS). We derive a simplified version of the model, which includes DMS as the sole parameter, in order to illuminate aspects of the migration process. Using this model, we show that the progressive phase alignment of MSA and Na+ concentration peaks observed along a high-resolution West Antarctic core is most consistent with 10−12m2s−1〈DMS〈10−11m2s−1, which is 1 order of magnitude greater than the DMS values previously estimated from laboratory studies. More generally, our data synthesis and model results suggest that (i) MSA migration may be fairly ubiquitous, particularly at coastal and (or) high-accumulation regions across Greenland and Antarctica; and (ii) can significantly change annual and multiyear MSA concentration averages. Thus, in most cases, caution should be exercised when interpreting polar ice core MSA records, although records that have undergone severe migration could still be useful for inferring decadal and lower-frequency climate variability.
    Print ISSN: 1994-0416
    Electronic ISSN: 1994-0424
    Topics: Geography , Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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