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| Home > Publications database > Probing structural homogeneity of La$_{1-x}$Gd$_{x}$PO$_{4}$ monazite-type solid solutions by combined spectroscopic and computational studies |
| Home > Publications database > Probing structural homogeneity of La$_{1-x}$Gd$_{x}$PO$_{4}$ monazite-type solid solutions by combined spectroscopic and computational studies |
| Journal Article | FZJ-2017-00893 |
; ; ; ; ;
2017
Elsevier Science
Amsterdam [u.a.]
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Please use a persistent id in citations: doi:10.1016/j.jnucmat.2017.01.024
Abstract: Here we study the homogeneity of Eu3+-doped La1-xGdxPO4 (x = 0, 0.11, 0.33, 0.55, 0.75, 0.92, 1) monazite-type solid solutions by a combination of Raman and time-resolved laser fluorescence spectroscopies (TRLFS) with complementary quasi-random structure-based atomistic modeling studies. For the intermediate La0.45Gd0.55PO4 composition we detected a significant broadening of the Raman bands corresponding to the lattice vibrations of the LnO9 polyhedron, indicating much stronger distortion of the lanthanide cation site than the PO4 tetrahedron. A distortion of the crystal lattice around the dopant site was also confirmed in our TRLFS measurements of Eu3+ doped samples, where both the half width (FWHM) of the excitation peaks and the 7F2/7F1 ratio derived from the emission spectra increase for intermediate solid-solution compositions. The observed variation in FWHM correlates well with the simulated distribution of Eu···O bond distances within the investigated monazites. The combined results imply that homogenous Eu3+-doped La1-xGdxPO4 monazite-type solid solutions are formed over the entire composition range, which is of importance in the context of using these ceramics for immobilization of radionuclides.
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