Titanium substitution mechanisms in forsterite

Ti K-edge X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectra, together with atomic scale calculations, indicate that Ti occupies the Si site in anhydrous forsterite. The energy and intensity of the 1s .3d transition in the XANES spectrum is diag...

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Main Authors: Berry, A., Walker, A., Herman, J., O'Neil, H., Foran, G., Gale, Julian
Format: Journal Article
Published: Elsevier Science BV 2007
Subjects:
Online Access:http://hdl.handle.net/20.500.11937/33653
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author Berry, A.
Walker, A.
Herman, J.
O'Neil, H.
Foran, G.
Gale, Julian
author_facet Berry, A.
Walker, A.
Herman, J.
O'Neil, H.
Foran, G.
Gale, Julian
author_sort Berry, A.
building Curtin Institutional Repository
collection Online Access
description Ti K-edge X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectra, together with atomic scale calculations, indicate that Ti occupies the Si site in anhydrous forsterite. The energy and intensity of the 1s .3d transition in the XANES spectrum is diagnostic of Ti on a four-coordinate site. The EXAFS spectra determine a Ti-O bond length of 1.81 0.01 This value is in excellent agreement with that of 1.8 A determined computationally by periodic density functional theory and an embedded cluster approach for Ti on the Si site; the calculated bond length for Ti on a Mg site is 2.0 Both computational methods further find that the direct substitution of Ti for Si is energetically favoured relative to substitution of Ti for Mg, charge balanced by either a Mg vacancy or Mg on a Si site. Together the results provide unambiguous evidence for Ti occupying the Si site in anhydrous forsterite. Ti-bearing olivine synthesised at upper mantle conditions in the presence of water, however, exhibits a pre-edge feature corresponding to six-fold coordination. This is consistent with the identification of a Ti-clinohumite-like point defect in samples of olivine from upper-mantle spinel peridotite. The change in Ti site thus provides a mechanism for the incorporation of water in olivine. The total Ti content of olivine will comprise varying contributions from Mg2 [4]TiO4 and Ti-clinohumite-like Mg[6]TiO2(OH)2 substitutions.
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spelling curtin-20.500.11937-336532018-03-29T09:08:14Z Titanium substitution mechanisms in forsterite Berry, A. Walker, A. Herman, J. O'Neil, H. Foran, G. Gale, Julian hydrous defects Nominally anhydrous minerals Density functional theory XANES EXAFS Forsterite Ti K-edge X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectra, together with atomic scale calculations, indicate that Ti occupies the Si site in anhydrous forsterite. The energy and intensity of the 1s .3d transition in the XANES spectrum is diagnostic of Ti on a four-coordinate site. The EXAFS spectra determine a Ti-O bond length of 1.81 0.01 This value is in excellent agreement with that of 1.8 A determined computationally by periodic density functional theory and an embedded cluster approach for Ti on the Si site; the calculated bond length for Ti on a Mg site is 2.0 Both computational methods further find that the direct substitution of Ti for Si is energetically favoured relative to substitution of Ti for Mg, charge balanced by either a Mg vacancy or Mg on a Si site. Together the results provide unambiguous evidence for Ti occupying the Si site in anhydrous forsterite. Ti-bearing olivine synthesised at upper mantle conditions in the presence of water, however, exhibits a pre-edge feature corresponding to six-fold coordination. This is consistent with the identification of a Ti-clinohumite-like point defect in samples of olivine from upper-mantle spinel peridotite. The change in Ti site thus provides a mechanism for the incorporation of water in olivine. The total Ti content of olivine will comprise varying contributions from Mg2 [4]TiO4 and Ti-clinohumite-like Mg[6]TiO2(OH)2 substitutions. 2007 Journal Article http://hdl.handle.net/20.500.11937/33653 10.1016/j.chemgeo.2007.03.010 Elsevier Science BV restricted
spellingShingle hydrous defects
Nominally anhydrous minerals
Density functional theory
XANES
EXAFS
Forsterite
Berry, A.
Walker, A.
Herman, J.
O'Neil, H.
Foran, G.
Gale, Julian
Titanium substitution mechanisms in forsterite
title Titanium substitution mechanisms in forsterite
title_full Titanium substitution mechanisms in forsterite
title_fullStr Titanium substitution mechanisms in forsterite
title_full_unstemmed Titanium substitution mechanisms in forsterite
title_short Titanium substitution mechanisms in forsterite
title_sort titanium substitution mechanisms in forsterite
topic hydrous defects
Nominally anhydrous minerals
Density functional theory
XANES
EXAFS
Forsterite
url http://hdl.handle.net/20.500.11937/33653