Pushing the limits: Resolving paleoseawater signatures in nanoscale fluid inclusions by atom probe tomography

Taylor, Sandra D.; Gregory, Daniel D.; Perea, Daniel E.; Kovarik, Libor; Cliff, John B.; Lyons, Timothy W.

doi:10.1016/j.epsl.2022.117859

Pushing the limits: Resolving paleoseawater signatures in nanoscale fluid inclusions by atom probe tomography

Journal Article · Wed Oct 12 00:00:00 EDT 2022 · Earth and Planetary Science Letters

DOI:https://doi.org/10.1016/j.epsl.2022.117859· OSTI ID:1897518

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Univ. of Toronto, ON (Canada)
Univ. of California, Riverside, CA (United States)

New insight into the geochemistry of ancient environments can be gained through structural and chemical analyses of nanometer-scale features within minerals. Here, we present recent developments using atom probe tomography (APT) enabling direct visualization of nanoscale fluid inclusions trapped within pyrite (FeS₂) and thereby chemical characterization of remnant seawater. Pyrite framboids (spherical clusters of nanocrystals) were sampled from the Middle Devonian Leicester Pyrite Member (New York). Scanning transmission electron microscopy shows low density regions distributed within the pyrite consistent with nanoscale pores (<4 nm in size). APT 3D visualization and compositional mapping reveals that the nanopores are filled with water. The inclusions appear to preserve the elemental signature of the water column in which the framboids formed, specifically seawater components including Na, K, Mg, and Ca. Mg/Ca ratios within the pyrite were generally measured to be within 0.6±0.2 – consistent with calcite-dominated seawater conditions existing in the Middle Devonian. Furthermore, this study demonstrates the potential for a novel approach to reconstruct paleoenvironmental conditions from coupled elemental and structural analyses of nanoscale fluid inclusions.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1897518

Alternate ID(s):: OSTI ID: 1960656

Report Number(s):: PNNL-SA-172856

Journal Information:: Earth and Planetary Science Letters, Journal Name: Earth and Planetary Science Letters Vol. 599; ISSN 0012-821X

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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