High-resolution photoluminescence spectroscopy employing Eu3+ as the structural probe unambiguously revealed a universal breakdown of crystallographic site symmetry in lanthanide-doped disordered crystals. The spectroscopic site symmetries of Eu3+ descend from crystallographic Oh to Cs (or C2) in α-NaYF4, and from crystallographic C3h to Cs in β-NaYF4, which were further verified by crystal-field level fitting.
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