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Iron sites in radiation-damaged allanite-(Ce): the effects of thermally induced oxidation and structural reorganization

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Abstract

Radiation-damaged allanite-(Ce) starts to recrystallize at an annealing temperature below 700 K. At the same temperature Fe2+ → Fe3+ oxidation, as well as dehydration occurs. Three radiation-damaged samples (S74 20414: 0.55 wt% ThO2, LB-1: 1.18 wt% ThO2, R1: 1.59 wt% ThO2) as well as one crystalline sample (RS221) were investigated using 57Fe Mössbauer spectroscopy after step-wise annealing. Additionally, the three damaged samples were investigated by in-situ mass spectrometry, analysing the escaping gases during thermal treatment showing the dehydration process. 57Fe Mössbauer spectroscopy revealed not only a general Fe2+ → Fe3+ oxidation, it also showed that this process is not fully completed after annealing at 1000 K in sample LB-1 which is the sample showing the fastest and strongest recrystallization. The crystalline sample also still incorporated Fe2+ as well as Fe3+ after annealing at 1000 K. In addition, a preferred occupation of iron at the position M3 was identified in the crystalline sample which did not occur in the pristine radiation-damaged samples (M1/M3 site distribution: RS221: 17/83, pristine samples R1: 49/51, LB-1: 60/40, S74 20414: 52/48). After annealing at 1000 K sample LB-1 showed a similar distribution as the crystalline sample with a M1/M3 distribution of 15/85. It is therefore proposed that the process of amorphization through α-decay damage changes the distribution of iron atoms on its possible crystallographic sites, and that this process is reversible through thermal annealing.

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Acknowledgments

This research was funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - BE 5456/2-1. We thank Radek Škoda, Jan Cempírek, and the Fersman Mineralogy Museum for samples.

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Authors and Affiliations

  1. Martin-Luther-University, Von-Seckendorff-Platz 3, Halle/Saale, 06120, Germany

    Claudia Eva Reissner, Herbert Pöllmann & Tobias Beirau

  2. TU Wien, Wiedner Hauptstraße 8-10, 1040, Wien, Austria

    Michael Reissner & Daniel Kern

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  1. Claudia Eva Reissner
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  2. Michael Reissner
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  4. Herbert Pöllmann
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Correspondence to Claudia Eva Reissner.

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This article is part of the Topical Collection on Proceedings of the International Conference on the Applications of the Mössbauer Effect (ICAME2019), 1-6 September 2019, Dalian, China

Edited by Tao Zhang, Junhu Wang and Xiaodong Wang

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Reissner, C.E., Reissner, M., Kern, D. et al. Iron sites in radiation-damaged allanite-(Ce): the effects of thermally induced oxidation and structural reorganization. Hyperfine Interact 241, 18 (2020). https://doi.org/10.1007/s10751-019-1686-4

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  • DOI: https://doi.org/10.1007/s10751-019-1686-4

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