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Supplementary Material This manuscript is provided as a supplementary material for the review process only
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| bet | 10/21 | | Sana | 01.08.2021 | | Hajmi | 8.05 Mb. | | #16503 |
Valence Electron Spectra Range. The valence bands of the studied samples were observed in the BE range 0 - ~35 eV. They consist of the OVMO (0 - ~15 eV BE) and IVMO (~15 - ~35 eV BE) ranges,42 (Figure 3). Peaks in the U 6p – O 2s BE range are relatively wide and structured comparing to the corresponding core U 4f and O 1s ones (Table 3, Figures 5 and 6). This contradicts the Heisenberg uncertainty ratio ΔEΔτ ≈ h/2π, where ΔE is the natural width of a level from which an electron was extracted, Δτ is the hole lifetime and h is the Planck constant. Since the hole lifetime (Δτ) grows as the absolute atomic level energy decreases, the lower BE XPS atomic peaks are expected to be narrower. In particular, if the O 2s level was atomic, its FWHM would be lower than that of the O 1s peak being Γ(O 1s)=1.0 eV (Table 3, Figure 5), which contradicts the experimental data. Taking into account the data on UO2 (refs 42 and 45), the O 2s and U 6p levels were shown not to be atomic, but the IVMO-related. The calculated results of the electronic structure of the cluster UO812-, representing uranium close environment in UO2, are presented under the spectrum of valence electrons (Figure 3). These results were obtained in approximation of the relativistic method of discrete variation (RDV).42
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