Development of routines for simultaneous in situ chemical composition and stable Si isotope ratio analysis by femtosecond laser ablation inductively coupled plasma mass spectrometry

Frick, Daniel A.; Schuessler, Jan A.; Blanckenburg, Friedhelm von

doi:10.1016/j.aca.2016.08.029

Cited by 27 publications

(19 citation statements)

References 40 publications

(75 reference statements)

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“…In-situ Si stable isotope-and the chemical composition of metal and silicate phases of chondrules, a metal-troilite spherule and matrix were determined using a laser ablation split stream (LASS) method (Glaus et al, 2013;Frick et al, 2016). A custom-built deep-UV (196 nm) femtosecond laser ablation system (GFZ fem2, a frequency-quadrupled Spectra Physics Solstice femtosecond laser, see Schuessler and Blanckenburg, 2014 for more details about the laser) was used to produce sample aerosol in a He gas stream.…”

Section: Mass Spectrometrymentioning

confidence: 99%

The origin of unequilibrated EH chondrites – Constraints from in situ analysis of Si isotopes, major and trace elements in silicates and metal

Kadlag

Tatzel

Frick

et al. 2019

Geochimica et Cosmochimica Acta

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Various lines of evidence suggest that material isotopically similar to enstatite chondrites may have accreted to the terrestrial planets. However, the enrichment of light Si isotopes in bulk enstatite chondrites is not easy to reconcile with the heavy Si isotopic composition of the Bulk Silicate Earth (BSE). To investigate the origin of the light Si isotopic composition of enstatite chondrites, we have obtained in-situ Si isotope data and simultaneously major-and trace element data in silicate and metal phases of chondrules, a metal-troilite spherule, and matrix from the enstatite chondrites Sahara 97072 (EH3) and Indarch (EH4) using laser ablation split stream-ICP-MS, which combines femto-second LA-MC-ICP-MS and Quadrupole-ICP-MS. Silicates in chondrules show variations in δ 30 Si (‰ variations of 30 Si/ 28 Si relative to NBS-28) ranges from-1.06 ± 0.13‰ (2 S.E.) to-0.38 ± 0.11‰. δ 30 Si in matrix silicates ranges from-0.96 ± 0.18‰ to-0.22 ± 0.12‰. The δ 30 Si-value of silicate phases varies independently of Mg/Si, ruling out simple equilibrium condensation from nebular gas. Some silicates in both enstatite chondrites have δ 30 Si-values like CI chondrites, whereas Si in other silicates is isotopically lighter, suggesting that the precursor materials of EH chondrites were already depleted in heavy Si isotopes. The metal phases in the matrix show average δ 30 Si of-6.0 ± 0.6‰. In spite of different metamorphic grades, the fractionation of Si isotopes between matrix metal and silicates in Sahara 97072 and Indarch shows no systematic differences, and thus no re-equilibration of Si 2 isotopes occurred between silicates and metal at metamorphic temperatures below 900 K. The δ 30 Si-value of metal from a metal-troilite spherule from Sahara 97072 (-8.24 ± 0.12‰) is lower than that of matrix metals. These differences were likely inherited from different formation environments of matrix-and spherule metal. If metal formation occurred under equilibrium conditions, then matrix metal may have formed at higher temperatures than the MTS metal. or at similar temperatures but slightly lower oxygen fugacities, or the MTS metal equilibrated with gas or silicates which were not incorporated into EH chondrites because they were lost from the EH chondrite formation region. Alternatively, the differences in δ 30 Si of different metals could also reflect variable kinetic isotope fractionation during the formation of metal and exsolution of perryite. The considerably lower δ 30 Si-values of bulk EH chondrites compared to CI-and other chondrites partly reflects the presence of Si bearing metal with isotopically light Si and partly silicates with isotopically light Si. The latter indicate loss of a heavy Si-rich silicate component from the EH3 formation region, presumably together with refractory elements. Although the Si isotopic composition of bulk EH chondrites precludes that these represent major building material of the Earth, the combination of complementary heavy Si isotope-and refractory element-enriched reduced materials and ca...

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Section: Mass Spectrometrymentioning

confidence: 99%

The origin of unequilibrated EH chondrites – Constraints from in situ analysis of Si isotopes, major and trace elements in silicates and metal

Kadlag

Tatzel

Frick

et al. 2019

Geochimica et Cosmochimica Acta

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“…An analytical protocol for accurate in situ Si isotope analysis has been established on a new second-generation custom-built femtosecond laser ablation system. The laser is coupled to a multicollector inductively coupled plasma mass spectrometer (fsLA-MC-ICP-MS) [75,76]. To resolve Si isotope signals from isobaric interferences (mainly 14 N 16 O polyatomic ions), the ion optics are operated in medium mass resolution mode, with which an external reproducibility better than ±0.23‰ (2σ) can be obtained.…”

Section: Analytical Techniquesmentioning

confidence: 99%

Silicon Isotope Geochemistry: Fractionation Linked to Silicon Complexations and Its Geological Applications

et al. 2019

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The fundamental advances in silicon isotope geochemistry have been systematically demonstrated in this work. Firstly, the continuous modifications in analytical approaches and the silicon isotope variations in major reservoirs and geological processes have been briefly introduced. Secondly, the silicon isotope fractionation linked to silicon complexation/coordination and thermodynamic conditions have been extensively stressed, including silicate minerals with variable structures and chemical compositions, silica precipitation and diagenesis, chemical weathering of crustal surface silicate rocks, biological uptake, global oceanic Si cycle, etc. Finally, the relevant geological implications for meteorites and planetary core formation, ore deposits formation, hydrothermal fluids activities, and silicon cycling in hydrosphere have been summarized. Compared to the thermodynamic isotope fractionation of silicon associated with high-temperature processes, that in low-temperature geological processes is much more significant (e.g., chemical weathering, biogenic/non-biogenic precipitation, biological uptake, adsorption, etc.). The equilibrium silicon isotope fractionation during the mantle-core differentiation resulted in the observed heavy isotope composition of the bulk silicate Earth (BSE). The equilibrium fractionation of silicon isotopes among silicate minerals are sensitive to the Si–O bond length, Si coordination numbers (CN), the polymerization degrees of silicate unites, and the electronegativity of cations in minerals. The preferential enrichment of different speciation of dissoluble Si (DSi) (e.g., silicic acid H4SiO40 (H4) and H3SiO4− (H3)) in silica precipitation and diagenesis, and chemical weathering, lead to predominately positive Si isotope signatures in continental surface waters, in which the dynamic fractionation of silicon isotope could be well described by the Rayleigh fractionation model. The role of complexation in biological fractionations of silicon isotopes is more complicated, likely involving several enzymatic processes and active transport proteins. The integrated understanding greatly strengthens the potential of δ30Si proxy for reconstructing the paleo terrestrial and oceanic environments, and exploring the meteorites and planetary core formation, as well as constraining ore deposits and hydrothermal fluid activity.

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“…We followed this procedure on reference materials of which the mean results and their uncertainties were compared with independently obtained δ 30 Si values and to verify the previously established target uncertainty of the fsLA‐MC‐ICP‐MS method of better than ± 0.23‰ (2 s ) and ± 0.15‰ (2 s ) for δ 30 Si and δ 29 Si, respectively (Schuessler and von Blanckenburg , Frick et al . ).…”

Section: Methodsmentioning

confidence: 97%

“…Instrumental mass bias was corrected for by calibrator‐sample bracketing using NIST SRM 610 as measurement standard (Frick et al . ). The laser beam ( ca .…”

Section: Methodsmentioning

confidence: 97%

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Laser Ablation In Situ Silicon Stable Isotope Analysis of Phytoliths

Frick

Schuessler

Sommer

et al. 2018

Geostandard Geoanalytic Res

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Silicon is a beneficial element for many plants and is deposited in plant tissue as amorphous bio-opal called phytoliths. The biochemical processes of silicon uptake and precipitation induce isotope fractionation: the mass-dependent shift in the relative abundances of the stable isotopes of silicon. At the bulk scale, d 30 Si ratios span from -2 to +6‰. To further constrain these variations in situ, at the scale of individual phytolith fragments, we used femtosecond laser ablation multicollector inductively coupled plasma-mass spectrometry (fsLA-MC-ICP-MS). A variety of phytoliths from grasses, trees and ferns were prepared from plant tissue or extracted from soil. Good agreement between phytolith d 30 Si ratios obtained by bulk solution MC-ICP-MS analysis and in situ isotope ratios from fsLA-MC-ICP-MS validates the method. Bulk solution analyses result in at least twofold better precision for d 30 Si (2s on reference materials ≤ 0.11‰) over that found for the means of in situ analyses (2s typically ≤ 0.24‰). We find that bushgrass, common reed and horsetail show large internal variations up to 2‰ in d 30 Si, reflecting the various pathways of silicon from soil to deposition. Femtosecond laser ablation provides a means to identify the underlying processes involved in the formation of phytoliths using silicon isotope ratios.

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Development of routines for simultaneous in situ chemical composition and stable Si isotope ratio analysis by femtosecond laser ablation inductively coupled plasma mass spectrometry

Cited by 27 publications

References 40 publications

The origin of unequilibrated EH chondrites – Constraints from in situ analysis of Si isotopes, major and trace elements in silicates and metal

The origin of unequilibrated EH chondrites – Constraints from in situ analysis of Si isotopes, major and trace elements in silicates and metal

Silicon Isotope Geochemistry: Fractionation Linked to Silicon Complexations and Its Geological Applications

Laser Ablation In Situ Silicon Stable Isotope Analysis of Phytoliths

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