Probing structural homogeneity of La 1-x Gd x PO 4  monazite-type solid solutions by combined spectroscopic and computational studies

Huittinen, Nina; Arinicheva, Yulia; Kowalski, Piotr M.; Vinograd, Victor L.; Neumeier, Stefan; Bosbach, Dirk

doi:10.1016/j.jnucmat.2017.01.024

Cited by 25 publications

(32 citation statements)

References 38 publications

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“…The results in combination with spectroscopic [54,193,215] and modeling studies [182,216] confirm the mismatch of ionic radii as well as the lattice strain to be responsible for the excess properties of these monazitetype solid solutions. Geisler et al [215], Neumeier et al [54] and Huittinen et al [193] observed a broadening in the Raman and laser fluorescence spectra of various monazite solid solutions. These observations are attributed to reflect lattice strain due to bond length distributions in the solid solutions.…”

Section: Bereitgestellt Von | Forschungszentrum Juelichsupporting

confidence: 55%

“…Very recently the excess enthalpy of mixing of La 1−x Ln x PO 4 (Ln = Pr, Eu, Gd) solid solutions were obtained from drop solution calorimetry [54,160]. The results in combination with spectroscopic [54,193,215] and modeling studies [182,216] confirm the mismatch of ionic radii as well as the lattice strain to be responsible for the excess properties of these monazitetype solid solutions. Geisler et al [215], Neumeier et al [54] and Huittinen et al [193] observed a broadening in the Raman and laser fluorescence spectra of various monazite solid solutions.…”

Section: Bereitgestellt Von | Forschungszentrum Juelichmentioning

confidence: 90%

“…Atomistic simulations have been found useful for the interpretation of the broadening of the laser fluorescence peak of Eu doped (La,Gd)-monazite-type solid solutions. Based on the simulation results, Huittinen et al [193] were able to explain the maximum broadening of the profiles observed for the intermediate solution compositions as the effect of distribution of the Eu-O bond lengths in the Eu-doped homogeneous (La,Gd)-solid solutions. This research provides a solid argument for the homogeneity of the solid solution.…”

Section: Progress In Atomistic Modeling Of Actinide-bearing Phosphatementioning

confidence: 99%

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New insights into phosphate based materials for the immobilisation of actinides

Neumeier

Arinicheva

et al. 2017

Radiochimica Acta

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This paper focuses on major phosphate-based ceramic materials relevant for the immobilisation of Pu, minor actinides, fission and activation products. Key points addressed include the recent progress regarding synthesis methods, the formation of solid solutions by structural incorporation of actinides or their non-radioactive surrogates and waste form fabrication by advanced sintering techniques. Particular attention is paid to the properties that govern the long-term stability of the waste forms under conditions relevant to geological disposal. The paper highlights the benefits gained from synergies of state-of-the-art experimental approaches and advanced atomistic modeling tools for addressing properties and stability of f-element-bearing phosphate materials. In conclusion, this article provides a perspective on the recent advancements in the understanding of phosphate based ceramics and their properties with respect to their application as nuclear waste forms.

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Section: Bereitgestellt Von | Forschungszentrum Juelichsupporting

confidence: 55%

Section: Bereitgestellt Von | Forschungszentrum Juelichmentioning

confidence: 90%

Section: Progress In Atomistic Modeling Of Actinide-bearing Phosphatementioning

confidence: 99%

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New insights into phosphate based materials for the immobilisation of actinides

Neumeier

Arinicheva

et al. 2017

Radiochimica Acta

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“…RW-1 fragments are transparent, but occasionally opaque with some fractures and inclusions under transmitted and reflected light (Appendix A, Figure A1). It has four main Raman bands at approximately 470, 620, 970, and 1050 cm −1 (Figure 1), typical of internal modes of the noninteracting PO 4 units within the monazite system [36,37]. The RW-1 Raman shift was consistent with those of UNIL-Mnz1, USGS-44069, and Manangoutry monazite standards (Figure 1).…”

Section: Rw-1 Mineralogical Features and Elemental Compositionsmentioning

confidence: 58%

“…The high-resolution X-ray map indicates that RW-1 is homogeneous without discernible Si, Th, Ce, or Y compositional zonation (Appendix A, Figure A1). [36,37]. The UNIL-Mnz1 and Diamantina monazite standards have an additional band at~990 cm −1 .…”

Section: Rw-1 Mineralogical Features and Elemental Compositionsmentioning

confidence: 99%

Further Characterization of the RW-1 Monazite: A New Working Reference Material for Oxygen and Neodymium Isotopic Microanalysis

Ling

et al. 2019

Minerals

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The oxygen (O) and neodymium (Nd) isotopic composition of monazite provides an ideal tracer of metamorphism and hydrothermal activity. Calibration of the matrix effect and monitoring of the external precision of monazite O–Nd isotopes with microbeam techniques, such as secondary ion mass spectrometry (SIMS) and laser ablation-multicollector-inductively coupled plasma-mass spectrometry (LA-MC-ICPMS), require well-characterized natural monazite standards for precise microbeam measurements. However, the limited number of standards available is impeding the application of monazite O–Nd isotopes. Here, we report on the RW-1 monazite as a potential new working reference material for microbeam analysis of O–Nd isotopes. Microbeam measurements by electron probe microanalysis (EPMA), SIMS, and LA-MC-ICPMS at 10–24 µm scales have confirmed that it is homogeneous in both elemental and O–Nd isotopic compositions. SIMS measurements yield δ18O values consistent, within errors, with those obtained by laser fluorination techniques. Precise analyses of Nd isotope by thermal ionization mass spectrometry (TIMS) are consistent with mean results of LA-MC-ICPMS analyses. We recommend δ18O = 6.30‰ ± 0.16‰ (2SD) and 143Nd/144Nd = 0.512282 ± 0.000011 (2SD) as being the reference values for the RW-1 monazite.

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Local Structural Effects of Eu³⁺ Incorporation into Xenotime‐type Solid Solutions with Different Host Cations

Xiao

Lösch

Huittinen

et al. 2018

Chemistry A European J

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In this study, the effect of host cations on the local structure around the dopant site of materials from the xenotime family is systematically studied on the molecular level. A series of six Eu -doped xenotime-type single crystals (Tb, Y, Ho, Er, Yb, and LuPO ) have been grown and spectroscopically analyzed by using polarization-dependent laser-induced luminescence spectroscopy (p-TRLFS). Our results demonstrate that the structural disorder changes in a non-linear manner with a structural break between Yb and Lu . Despite adopting identical crystal structures, the solid solutions of these materials vary significantly, and differ from monazite solid solutions. Similar Eu incorporation behavior with a strongly distorted dopant site is found for the early members of the xenotime family, whereas LuPO with the largest host versus dopant radii mismatch is anomalous in that it contains the most symmetrical lattice site. This goes along with a significantly stronger crystal field, indicating a shorter Eu-O bond length, as well as a strong vibronic coupling to external translational lattice vibrations. The p-TRLFS analysis confirms the breakdown of the crystallographic site symmetry from D to C in YPO , whereas a small distortion of the crystallographic site in LuPO results in an S point symmetry for the Eu cation. The lattice with the smallest cation host site is no longer sufficiently flexible to make room for Eu and instead "forces" the guest ion to occupy a less distorted Lu site.

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Probing structural homogeneity of La 1-x Gd x PO 4 monazite-type solid solutions by combined spectroscopic and computational studies

Cited by 25 publications

References 38 publications

New insights into phosphate based materials for the immobilisation of actinides

New insights into phosphate based materials for the immobilisation of actinides

Further Characterization of the RW-1 Monazite: A New Working Reference Material for Oxygen and Neodymium Isotopic Microanalysis

Local Structural Effects of Eu³⁺ Incorporation into Xenotime‐type Solid Solutions with Different Host Cations

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Probing structural homogeneity of La 1-x Gd x PO 4 monazite-type solid solutions by combined spectroscopic and computational studies

Cited by 25 publications

References 38 publications

New insights into phosphate based materials for the immobilisation of actinides

New insights into phosphate based materials for the immobilisation of actinides

Further Characterization of the RW-1 Monazite: A New Working Reference Material for Oxygen and Neodymium Isotopic Microanalysis

Local Structural Effects of Eu3+ Incorporation into Xenotime‐type Solid Solutions with Different Host Cations

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Local Structural Effects of Eu³⁺ Incorporation into Xenotime‐type Solid Solutions with Different Host Cations