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

S. D. Taylor; D. D. Gregory; D. E. Perea; L. Kovarik; J. B. Cliff; T. W. Lyons

doi:10.1016/j.epsl.2022.117859

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

S. D. Taylor, D. D. Gregory, D. E. Perea, L. Kovarik, J. B. Cliff, T. W. Lyons

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

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 features distributed within the pyrite (<4 nm in size). Three-dimensional chemical visualization and analysis by APT reveals these to be nanoscale fluid inclusions preserving the elemental signatures of the water column in which the framboids formed, as alkalis consistent with seawater including Na, K, Mg, and Ca are identified. Further, within the inclusions Mg/Ca is measured to be ∼0.6±0.2 – consistent with conditions for calcite-dominated seawater existing in the Middle Devonian. The results and approach developed in this study show the potential to reconstruct paleoenvironmental conditions from coupled elemental and structural analyses of nanoscale fluid inclusions.

Original language	English
Article number	117859
Journal	Earth and Planetary Science Letters
Volume	599
DOIs	https://doi.org/10.1016/j.epsl.2022.117859
State	Published - Dec 1 2022
Externally published	Yes

Funding

Sample preparation and LEAP 4000 XHR analyses were performed on a project award ( doi.org/10.46936/sthm.proj.2017.49860/60006201 ) from the Environmental Molecular Sciences Laboratory, a DOE Office of Science User Facility sponsored by the Biological and Environmental Research program under Contract No. DE-AC05-76RL01830 and located at PNNL. We thank Jeffery Over and Stephanie Olson for help during sample of the Leicester pyrite member. We further acknowledge funding through an NSERC Discovery Grant # 04843 funding to Gregory.

Keywords

atom probe tomography
fluid inclusion
pyrite
seawater chemistry

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10.1016/j.epsl.2022.117859

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title = "Pushing the limits: Resolving paleoseawater signatures in nanoscale fluid inclusions by atom probe tomography",

abstract = "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 features distributed within the pyrite (<4 nm in size). Three-dimensional chemical visualization and analysis by APT reveals these to be nanoscale fluid inclusions preserving the elemental signatures of the water column in which the framboids formed, as alkalis consistent with seawater including Na, K, Mg, and Ca are identified. Further, within the inclusions Mg/Ca is measured to be ∼0.6±0.2 – consistent with conditions for calcite-dominated seawater existing in the Middle Devonian. The results and approach developed in this study show the potential to reconstruct paleoenvironmental conditions from coupled elemental and structural analyses of nanoscale fluid inclusions.",

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author = "Taylor, {S. D.} and Gregory, {D. D.} and Perea, {D. E.} and L. Kovarik and Cliff, {J. B.} and Lyons, {T. W.}",

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AU - Perea, D. E.

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AU - Lyons, T. W.

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AB - 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 features distributed within the pyrite (<4 nm in size). Three-dimensional chemical visualization and analysis by APT reveals these to be nanoscale fluid inclusions preserving the elemental signatures of the water column in which the framboids formed, as alkalis consistent with seawater including Na, K, Mg, and Ca are identified. Further, within the inclusions Mg/Ca is measured to be ∼0.6±0.2 – consistent with conditions for calcite-dominated seawater existing in the Middle Devonian. The results and approach developed in this study show the potential to reconstruct paleoenvironmental conditions from coupled elemental and structural analyses of nanoscale fluid inclusions.

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

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