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231Pa, 230Th and 232Th as tracers of deep water circulation and particle transport: Insights from the Mediterranean Sea and the Arctic Ocean
Stockholm University, Faculty of Science, Department of Geological Sciences.ORCID iD: 0000-0003-2057-5795
2020 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The naturally occurring U and Th-series radionuclides have shown to have a considerable importance for the understanding of biogeochemical processes on Earth and in the ocean. In this thesis, the isotopes 230-thorium (230Th), 232-thorium (232Th) and 231-protactinium (231Pa) are used as tracers of the transport and scavenging of marine particles and water circulation. Pa and Th are particle reactive elements, which makes the production, transport and distribution of Pa and Th key factors for our understanding of the origin, fate and distribution of marine particles in the oceans. 

This thesis explores the distribution of 231Pa, 230Th and 232Th in two different ocean continental margin environments. In particular, the relative influence of water circulation and particles on the 231Pa, 230Th and 232Th distributions in the Arctic Ocean and Mediterranean Sea was investigated. 231Pa, 230Th and 232Th were analyzed in particles and seawater collected in the Mediterranean Sea during the MedSeA-GA04-S cruise along the GEOTRACES section GA04S and in the Arctic Ocean during the PS94 GN04 ARK-XXIX/3 along the GEOTRACES section GN04.

One of the important findings of this thesis was the low fractionation between 231Pa and 230Th in the Mediterranean Sea, contrasting what is observed in the open ocean. Additionally, the observed depth profiles of Pa-Th allowed the identification of deep water convection and ventilation in the Western and Eastern Basins, respectively. Moreover, the particle settling speed was reevaluated to ~500 – 1000 m/y.

In the Arctic Ocean, scavenging onto particles derived from hydrothermal activity was producing relatively low F-factors (FTh/Pa ~ 10), while higher values were observed in deep waters (FTh/Pa ~ 20). Additionally, the hydrothermal particles in the Nansen interior produce lower FTh/Pa values compared to FTh/Pa observed at the Nansen continental margin. Application of a boundary scavenging model revealed the importance of 230Th scavenging at the continental margin along the Nansen Basin, hereafter the Nansen margin, and advocate for the advection of 231Pa into the Atlantic Ocean. As the ocean margin was included in this model, a particle settling speed of 600 m/y was obtained at the Nansen margin.

Moreover, this thesis includes an inter-comparison of dissolved and particulate 231Pa, 230Th and 232Th measurements between four laboratories of the GEOTRACES community. This comparison was conducted to provide detailed descriptions of various chemical procedures used for Pa-Th analysis and to provide a measure of consistency between the laboratories. Results demonstrated that participating labs can determine concentrations of dissolved 230Th and 231Pa in deep water (below 500 m depth) that are internally consistent within 4 % of the mean values. Analysis of particulate 231Pa, 230Th and 232Th allowed the highlighting of an incomplete Pa dissolution problem with our initial leaching procedure, a problem solved by measuring aliquots of particulate samples at two labs. However, in the present work, consistent particulate 231Pa concentrations as low as ~ 0.002 fg/kg were obtained. Overall, it suggests an improvement of the results consistency compared to the previous GEOTRACES intercalibration exercise.

Place, publisher, year, edition, pages
Stockholm: Department of Geological Sciences, Stockholm University , 2020.
Series
Meddelanden från Stockholms universitets institution för geologiska vetenskaper ; 381
Keywords [en]
protactinium, thorium, Mediterranean Sea, Arctic Ocean, scavenging, marine particles, boundary scavenging, particle transport, geotraces
National Category
Geochemistry
Research subject
Marine Geology
Identifiers
URN: urn:nbn:se:su:diva-185750ISBN: 978-91-7911-319-3 (print)ISBN: 978-91-7911-320-9 (electronic)OAI: oai:DiVA.org:su-185750DiVA, id: diva2:1475333
Public defence
2020-12-11, William-Olssonsalen, Geovetenskapens hus, Svante Arrhenius väg 14, digitally via conference (Zoom), public link https://stockholmuniversity.zoom.us/j/63684779967, Stockholm, 10:00 (English)
Opponent
Supervisors
Projects
geotracesMedSeA
Funder
Swedish Polar Research SecretariatSwedish Research Council, VR 349-202-6287Available from: 2020-11-18 Created: 2020-10-12 Last updated: 2022-02-25Bibliographically approved
List of papers
1. Thorium and protactinium isotopes as tracers of marine particle fluxes and deep water circulation in the Mediterranean Sea
Open this publication in new window or tab >>Thorium and protactinium isotopes as tracers of marine particle fluxes and deep water circulation in the Mediterranean Sea
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2018 (English)In: Marine Chemistry, ISSN 0304-4203, E-ISSN 1872-7581, Vol. 199, p. 12-23Article in journal (Refereed) Published
Abstract [en]

231Pa, 230Th and 232Th were analyzed in unfiltered seawater samples (n =66) and suspended particles (n =19)collected in the Mediterranean Sea during the MedSeA-GA04-S cruise along the GEOTRACES section GA04S andused to investigate mechanisms controlling the distribution and fractionation of Pa and Th in an ocean marginenvironment. 231Pa and 230Th are particle reactive radionuclides and are often used as tracers of processes suchas boundary scavenging, particle transport and ocean circulation. The depth profiles of total 231Pa and 230Thconcentrations in the Mediterranean Sea displayed non-linear shapes. Higher total 232Th concentrations wereobserved at the straits and in deep waters pointing at lithogenic sources. Fractionation factors FTh/Pa ranged from1.4 to 9. Application of a box-model illustrated that 94% of the 231Pa and almost all of the 230Th (99.9%)produced in the Mediterranean Sea is removed to the sediment by scavenging. The negligible export of 230Th tothe Atlantic Ocean, leads to a reevaluation of the mean settling speed of the filtered particles, which is nowestimated to 500–1000 m/y. The low FTh/Pa fractionation factors are attributed to the efficient scavenging andlack of transport of 231Pa to the Atlantic Ocean.

National Category
Geochemistry
Research subject
Marine Geology
Identifiers
urn:nbn:se:su:diva-185827 (URN)10.1016/j.marchem.2017.12.002 (DOI)000426223600002 ()
Projects
GEOTRACES
Funder
Swedish Research Council, 349- 202-6287
Available from: 2020-10-12 Created: 2020-10-12 Last updated: 2022-07-12Bibliographically approved
2. 231Pa and 230Th in the Arctic Ocean: Implications for boundary scavenging and 231Pa-230Th fractionation in the Eurasian Basin
Open this publication in new window or tab >>231Pa and 230Th in the Arctic Ocean: Implications for boundary scavenging and 231Pa-230Th fractionation in the Eurasian Basin
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2020 (English)In: Chemical Geology, ISSN 0009-2541, E-ISSN 1872-6836, Vol. 532, article id 119380Article in journal (Refereed) Published
Abstract [en]

231Pa, 230Th and 232Th were analyzed in filtered seawater (n=70) and suspended particles (n=39) collectedalong a shelf-basin transect from the Barents shelf to the Makarov Basin in the Arctic Ocean during GEOTRACESsection GN04 in 2015. The distribution of dissolved 231Pa and 230Th in the Arctic Ocean deviates from the linearincrease expected from reversible scavenging. Higher 232Th concentrations were observed at the shelf, slope andin surface waters in the deep basin, pointing at lithogenic sources. Fractionation factors (FTh/Pa) observed at theNansen margin were higher compared to FTh/Pa in the central Nansen Basin, possibly due to the residual occurrenceof hydrothermal particles in the deep central Nansen Basin. Application of a boundary scavengingmodel quantitatively accounts for the dissolved and particulate 230Th distributions in the Nansen Basin.Modelled dissolved 231Pa distributions were largely overestimated, which was attributed to the absence of incorporation of water exchange with the Atlantic Ocean in the model. 231Pa/230Th ratios of the suspended particlesof the Nansen Basin were below the 231Pa/230Th production ratio, but top-core sediments of the Nansenmargin and slope have high 231Pa/230Th-ratios, suggesting that scavenging along the Nansen margin partly actsas a sink for the missing Arctic 231Pa.

Keywords
GEOTRACES, Protactinium, Thorium, Arctic Ocean, Boundary scavenging
National Category
Geochemistry
Research subject
Marine Geology
Identifiers
urn:nbn:se:su:diva-185828 (URN)10.1016/j.chemgeo.2019.119380 (DOI)000513868400001 ()
Projects
GEOTRACES
Funder
Swedish Research Council, 349- 202-6287
Available from: 2020-10-12 Created: 2020-10-12 Last updated: 2022-07-12Bibliographically approved
3. A comparison of dissolved and particulate 231Pa, 230Th and 232Th concentrations measured at the GEOTRACES Arctic crossover station in 2015
Open this publication in new window or tab >>A comparison of dissolved and particulate 231Pa, 230Th and 232Th concentrations measured at the GEOTRACES Arctic crossover station in 2015
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

The global mapping of the GEOTRACES program requires consistent and precise measurements of 232Th (pg/kg), 230Th and 231Pa (fg/kg) in seawater and suspended particulate matter. Concentrations of particulate and dissolved 231Pa, 230Th and 232Th were measured by four labs in samples collected at the Arctic crossover station in 2015. These samples were collected during two separate expeditions (HLY1502 GN01, Station 30 and PS94 GN04 ARK-XXIX/3, Station 101). Detailed descriptions of chemical procedures used by the participating labs are followed by a discussion focused on dissolved surface samples and particulate samples. Results demonstrated that participating labs can determine concentrations of dissolved 230Th and 231Pa in deep water (<500 m depth) that are internally consistent within 4 % of the mean values. However, the analysis of radionuclide concentrations in suspended particles still needs improvement. The pre-concentration of particulate material used at LSCE was proven to be unsuccessful. Aliquots of particulate samples at St. 101 were re-measured and it was concluded that the absence of HF in the leaching solution was the cause for the previously underestimated particulate concentrations. Large blank contributions are still a problem, especially for measurements of particulate 231Pa.

Keywords
GEOTRACES, Protactinium, Thorium, intercalibration, Arctic Ocean
National Category
Geochemistry
Research subject
Marine Geology
Identifiers
urn:nbn:se:su:diva-185829 (URN)
Projects
GEOTRACES
Funder
Swedish Research Council, 349-202-6287
Available from: 2020-10-12 Created: 2020-10-12 Last updated: 2022-07-12Bibliographically approved

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