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Nitrogen incorporation in silicates and metals: Results from SIMS, EPMA, FTIR, and laser-extraction mass spectrometry

  • Jed L. Mosenfelder EMAIL logo , Anette Von Der Handt , Evelyn Füri , Celia Dalou , Richard L. Hervig , George R. Rossman and Marc M. Hirschmann
Published/Copyright: January 2, 2019
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American Mineralogist
From the journal American Mineralogist Volume 104 Issue 1

Abstract

A quantitative understanding of nitrogen incorporation in Earth materials is important for constraining volatile evolution in planetary bodies. We used a combination of chemical (SIMS, EPMA, and laser-extraction mass spectrometry) and spectroscopic (FTIR) observations to study nitrogen contents and speciation mechanisms in silicate glasses, metal alloys, and an N-bearing silicate mineral (hyalophane). One suite of Fe-free basaltic glasses was studied by all four methods. Concentrations of N in these glasses determined by EPMA are systematically higher than those measured by laser extraction but agree within mutual 2s uncertainties, demonstrating the general veracity of the EPMA method. SIMS working curves based on measurement of 14N+ and 14N16O- as a function of N content determined by EPMA (or laser extraction) are best fit with exponential functions rather than the linear regressions that are most commonly applied to SIMS data. On the other hand, the relationship based on 12C14N- for C-poor, Fe-free glasses is exceptionally well fit to a linear regression (r2 = 1, p < 0.001), in contrast to expectations from previous work on glasses with lower N contents. Matrix effects on the SIMS signals associated with Fe or H2O content are not justified by the data, but volatile data (both N and H) for hyalophane, which contains 20 wt% BaO, reveal matrix effects possibly induced by its high average molar mass. A combination of FTIR and chemical data, together with a thorough review of the literature, was used to determine incorporation mechanisms for N in the Fe-free glasses. We infer that under reducing conditions at high pressure and temperature N is dissolved in basaltic melts chiefly as NH2−and NH2–, with N2 and/or nitride (X-N3–) complexes 2 becoming increasingly important at low fO2,increasing N content, and decreasing H content. Our results have implications for future studies seeking to accurately measure N by SIMS and for studies of N partitioning at high pressure relevant to planetary accretion and differentiation.

Keywords: SIMS; nitrogen; speciation; FTIR; EPMA; bonding; carbon

Acknowledgments

This work was supported by NSF grants EAR-1426772, AST-1344133, and EAR-1322082. The National ASU SIMS facility is supported by NSF EAR-1352996. We gratefully acknowledge Lynda Williams and Margo Regier for assistance with SIMS at ASU and Yunbin Guan for assistance with SIMS at Caltech. The manuscript was improved by reviews from Michael Wiedenbeck, associate editor Adam Kent, and an anonymous referee. We also thank Andrew Locock for providing the hyalophane sample. This paper is dedicated to Erik Hauri, who was an inspirational geochemist and a pioneer in the use of SIMS for measuring volatile elements in geological materials.

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Received: 2018-03-01
Accepted: 2018-09-07
Published Online: 2019-01-02
Published in Print: 2019-01-28

© 2019 Walter de Gruyter GmbH, Berlin/Boston

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  10. Nature of hydrogen defects in clinopyroxenes from room temperature up to 1000 °C: Implication for the preservation of hydrogen in the upper mantle and impact on electrical conductivity
  11. Phase transition boundary between fcc and hcp structures in Fe-Si alloy and its implications for terrestrial planetary cores
  12. Cathodoluminescence features, trace elements, and oxygen isotopes of quartz in unidirectional solidification textures from the Sn-mineralized Heemskirk Granite, western Tasmania
  13. Controls on cassiterite (SnO2) crystallization: Evidence from cathodoluminescence, trace-element chemistry, and geochronology at the Gejiu Tin District
  14. Anomalous elastic behavior of phase egg, AlSiO3(OH), at high pressures
  15. “Kamchatite” diamond aggregate from northern Kamchatka, Russia: New find of diamond formed by gas phase condensation or chemical vapor deposition
  16. An example of high-T, high-symmetry crystallization: Spherical (Mg,Fe)-oxides formed by particle attachment in the shocked martian meteorite Northwest Africa 7755
  17. Letter
  18. Zinc transport in hydrothermal fluids: On the roles of pressure and sulfur vs. chlorine complexing
  19. Book Review
  20. Book Review: Infrared and Raman Spectroscopies of Clay Minerals
https://doi.org/10.2138/am-2019-6533
Keywords for this article
SIMS; nitrogen; speciation; FTIR; EPMA; bonding; carbon

Articles in the same Issue

  1. Highlights and Breakthroughs
  2. Iron carbide in the core
  3. Reconstruction of residual melts from the zeolitized explosive products of alkaline-mafic volcanoes
  4. Inefficient high-temperature metamorphism in orthogneiss
  5. Nitrogen incorporation in silicates and metals: Results from SIMS, EPMA, FTIR, and laser-extraction mass spectrometry
  6. Activation of [100](001) slip system by water incorporation in olivine and the cause of seismic anisotropy decrease with depth in the asthenosphere
  7. In-situ high-temperature vibrational spectra for synthetic and natural clinohumite: Implications for dense hydrous magnesium silicates in subduction zones
  8. Stability of the hydrous phases of Al-rich phase D and Al-rich phase H in deep subducted oceanic crust
  9. Minerals in cement chemistry: A single-crystal neutron diffraction study of ettringite, Ca6Al2(SO4)3(OH)12·27H2O
  10. Nature of hydrogen defects in clinopyroxenes from room temperature up to 1000 °C: Implication for the preservation of hydrogen in the upper mantle and impact on electrical conductivity
  11. Phase transition boundary between fcc and hcp structures in Fe-Si alloy and its implications for terrestrial planetary cores
  12. Cathodoluminescence features, trace elements, and oxygen isotopes of quartz in unidirectional solidification textures from the Sn-mineralized Heemskirk Granite, western Tasmania
  13. Controls on cassiterite (SnO2) crystallization: Evidence from cathodoluminescence, trace-element chemistry, and geochronology at the Gejiu Tin District
  14. Anomalous elastic behavior of phase egg, AlSiO3(OH), at high pressures
  15. “Kamchatite” diamond aggregate from northern Kamchatka, Russia: New find of diamond formed by gas phase condensation or chemical vapor deposition
  16. An example of high-T, high-symmetry crystallization: Spherical (Mg,Fe)-oxides formed by particle attachment in the shocked martian meteorite Northwest Africa 7755
  17. Letter
  18. Zinc transport in hydrothermal fluids: On the roles of pressure and sulfur vs. chlorine complexing
  19. Book Review
  20. Book Review: Infrared and Raman Spectroscopies of Clay Minerals
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