Analysis and comparison of holmium 4f10energy levels in Cs2NaHoCl6and Cs2NaHoBr6

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Abstract
Energy level data recently reported for HoCl3- 6 and HoBr3- 6 in cubic elpasolite crystals are analysed in terms of a model hamiltonian that includes 20 ‘free-ion’ parameters and either two or four crystal-field interaction parameters. Each system is assumed to have octahedral (Oh ) site symmetry at the Ho3+ ions. Comparisons of the HoCl3- 6 and HoBr3- 6 systems are based on analyses of energy levels split out of the 5 IJ (J = 8, 7, 6, 5, and 4), 5 FJ (J = 5, 4, 3, and 2), and 5 S 2 multiplets of the 4f 10 electronic configuration of Ho3+. These analyses show that the Cl- ligands interact with the 4f electrons of Ho3+ somewhat more strongly than do the Br- ligands, and this difference in interactive strengths is exhibited most strongly in the sixth-rank crystal-field parameters. The empirical energy level data available for HoCl3- 6 (but not HoBr3- 6) spanned the 3 K 8, 7 and 5 G 6, 5 multiplet manifolds as well as the 5 IJ , 5 FJ , and 5 S 2 multiplets noted above. Analyses of these data show a rather striking term dependence of the phenomenological (‘fitted’) crystal-field parameters. They also suggest the possible importance of ‘spin-correlated crystal-field’ (SCCF) effects in the Cs2NaHoCl6 energy level structure. Estimates of SCCF contributions to the total crystal-field hamiltonian are reported.

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