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A Raman spectroscopic study on the structural disorder of monazite–(Ce)

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Abstract

This study addresses whether Raman spectra can be used to estimate the degree of accumulated radiation damage in monazite-(Ce) samples whose chemical composition was previously determined. Our results indicate that the degree of disorder in monazite–(Ce), as observed from increasing Raman band broadening, generally depends on both the structural state (i.e., radiation damage) and the chemical composition (i.e., incorporation of non-formula elements). The chemical effects were studied on synthetic orthophosphates grown using the Li-Mo flux method, and non radiation-damaged analogues of the naturally radiation-damaged monazite–(Ce) samples, produced by dry annealing. We found that the “chemical” Raman-band broadening of natural monazite–(Ce) can be predicted by the empirical formula,

$$ {\hbox{FWHM}} {\hbox{[c}}{{\hbox{m}}^{ - {1}}}{]} = {3}{.95} + {26}{.66} \times {\hbox{(Th}} + {\hbox{U}} + {\hbox{Ca}} + {\hbox{Pb)}} {\hbox{[apfu]}} $$

where, FWHM = full width at half maximum of the main Raman band of monazite–(Ce) (i.e., the symmetric PO4 stretching near 970 cm−1), and (Th+U+Ca+Pb) = sum of the four elements in apfu (atoms per formula unit). Provided the chemical composition of a natural monazite–(Ce) is known, this “chemical band broadening” can be used to estimate the degree of structural radiation damage from the observed FWHM of the ν1(PO4) band of that particular sample using Raman spectroscopy. Our annealing studies on a wide range of monazite–(Ce) reference materials and other monazite–(Ce) samples confirmed that this mineral virtually never becomes highly radiation damaged. Potential advantages and the practical use of the proposed method in the Earth sciences are discussed.

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Acknowledgements

The natural monazite–(Ce) samples used in this study were kindly made available by A. Ertl, M. J. Jercinovic, A. K. Kennedy, B. Schulz, and A.-M. Seydoux-Guillaume. Thanks are due to A. Wagner for sample preparation, and C. Fisher, E. Libowitzky and D. Talla for experimental assistance. Helpful comments by two anonymous reviewers and associate editor A. Beran are gratefully acknowledged. Partial funding for this research was provided by the European Commission through contract no. MEXC–CT–2005–024878 and the Austrian Science Fund (FWF) grant P20028–N10 to LN. DMT acknowledges the support by the Austrian Ministry of Science (BMWF) as part of the UniInfrastrukturprogramm of the Forschungsplattform Scientific Computing at LFU Innsbruck. JMH thanks the Canadian Natural Sciences and Research Council (NSERC) for partial support for this research in the form of a Discovery Grant, and Memorial University of Newfoundland, for additional financial support for this project.

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  1. Daniel M. Többens

    Present address: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Hahn-Meitner-Platz 1, 14109, Berlin, Germany

Authors and Affiliations

  1. Institut für Mineralogie und Kristallographie, Universität Wien, Althanstraße 14, 1090, Wien, Austria

    Katja Ruschel & Lutz Nasdala

  2. Geowissenschaftliches Zentrum, Universität Göttingen, Goldschmidtstr. 1, 37077, Göttingen, Germany

    Andreas Kronz

  3. Department of Earth Sciences, Memorial University of Newfoundland, St. John’s, NL, A1B 3X5, Canada

    John M. Hanchar

  4. Institut für Mineralogie und Petrographie, Universität Innsbruck, Innrain 52, 6020, Innsbruck, Austria

    Daniel M. Többens

  5. Institute of Geological Sciences, Masaryk University, Kotlářská 2, 61137, Brno, Czech Republic

    Radek Škoda

  6. Institut für Mineralogie, Universität Salzburg, Hellbrunnerstraße 34, 5020, Salzburg, Austria

    Friedrich Finger

  7. Department of Geology, University of Kansas, 1475 Jayhawk Boulevard, 120 Lindley Hall, Lawrence, KS, 66045-7613, USA

    Andreas Möller

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Ruschel, K., Nasdala, L., Kronz, A. et al. A Raman spectroscopic study on the structural disorder of monazite–(Ce). Miner Petrol 105, 41–55 (2012). https://doi.org/10.1007/s00710-012-0197-7

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