Abstract
Absorption and fluorescence spectra of Er3+(4f11) in crystals of NaBi(WO4)2 (NBW) are reported at temperatures between 15 K and room temperature. The absorption spectra include the details of the crystal-field splitting of 11 multiplet manifolds, LJ2S+1 of Er3+(4f11), spanning the wavelength range between 350 nm and 1550 nm. The crystal-field splitting of the ground-state I15/24, is obtained from an analysis of the fluorescence spectrum, S3/24→I15/24. Spectra are characterized by inhomogeneous broadening due to the disordered crystal structure in which different valency cations, Na+ and Bi3+, statistically fill the S4 symmetry sites. The Er3+ ions likely replace the Bi3+ ions in these sites. A quasi-center model has been chosen to interpret the crystal-field splitting of each manifold, using D2d rather than S4 symmetry as the site for the rare-earth ion in the lattice. To test the feasibility of the model, the splitting of the energy levels of Nd3+ in NBW was carried out first and compared with experimental levels reported in literature. A least-squares fitting analysis between 26 calculated-to-observed energy (Stark) levels gave a root-mean-square (rms) deviation of 8 cm−1 for the IJ4 and F3/24 multiplet manifolds of Nd3+ in NBW. Using the phenomenological lattice-sum parameters, Anm, obtained from the analysis of the Nd3+ energy levels, we predicted an initial set of crystal-field parameters, Bnm, for Er3+. With only a modest fitting of the multiplet centroids, these Bnm predict the observed splitting in the Er3+ spectra remarkably well. In a fitting of the energy levels in which both the Bnm and centroids are allowed to vary, we obtained a rms deviation of 6 cm−1 for 57 calculated-to-observed Stark levels. The results suggest that the quasi-center model has merit when used to calculate the crystal-field splitting of the energy levels of the trivalent rare-earth ions in crystal hosts having a disordered structure.
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