Technetium incorporation in scheelite: insights from first-principles

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Atomistic investigations of crystalline scheelite, CaWO4, and 99Tc-bearing scheelite, CaWO4:Tc, have been carried out using density functional theory. The lattice constants, bulk modulus, and volume compression data of CaWO4 have been calculated and compared with experimental data, with a focus on predictive understanding of 99Tc incorporation in CaWO4. Defect formation energies have been computed for several possible interstitial (I) and substitutional (S) sites of 99Tc in CaWO4. Both I(Oh) and S(W) sites were found to be energetically favourable for Tc doping. X-ray diffraction (XRD) spectra for each 99Tc defect type have been simulated to help interpret the complex experimental XRD patterns. This work on CaWO4:Tc provides insights into materials generated during nuclear weapons testing and useful spectral signatures for nuclear forensics. © The Royal Society of Chemistry.