Journal
FRONTIERS IN CHEMISTRY
Volume 7, Issue -, Pages -Publisher
FRONTIERS MEDIA SA
DOI: 10.3389/fchem.2019.00013
Keywords
xenotime YPO4; monazite LaPO4; nuclear waste forms; rare-earth elements REE; luminescence spectroscopy; grazing-incidence X-ray diffraction; amorphous fraction; structural disorder
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Funding
- ARC CFSS/GEMOC atMacquarie University, Sydney
- Austrian Science Fund (FWF) [J3662-N19]
- Austrian Science Fund (FWF) [J 3662] Funding Source: researchfish
- Austrian Science Fund (FWF) [J3662] Funding Source: Austrian Science Fund (FWF)
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In this study, we present a new concept based on the steady-state, laser-induced photoluminescence of Nd3+, which aims at a direct determination of the amorphous fraction f(a) in monazite- and xenotime-type orthophosphates on a micrometer scale. Polycrystalline, cold-pressed, sintered LaPO4, and YPO4 ceramics were exposed to quadruple Au-ion irradiation with ion energies 35 MeV (50% of the respective total fluence), 22 MeV (21%), 14 MeV (16%), and 7 MeV (13%). Total irradiation fluences were varied in the range 1.6 x 10(13)-6.5 x 10(13) ions/cm(2). Ion-irradiation resulted in amorphization and damage accumulation unto a depth of similar to 5 mu m below the irradiated surfaces. The amorphous fraction created was quantified by means of surface-sensitive grazing-incidence X-ray diffraction and photoluminescence spectroscopy using state-of-the-art confocal spectrometers with spatial resolution in the mu m range. Monazite-type LaPO4 was found to be more susceptible to ion-irradiation induced damage accumulation than xenotime-type YPO4. Transmission electron microscopy of lamella cut from irradiated surfaces with the focused-ion beam technique confirmed damage depth-profiles with those obtained from PL hyperspectral mapping. Potential analytical advantages that arise from an improved characterization and quantification of radiation damage (i.e., f(a)) on the mu m-scale are discussed.
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