The optical spectra of the lanthanides doped into single crystal LaF3 have been interpreted in terms of transitions within 4f N configurations. Energy matrices combining free‐ion terms with a crystal field for an approximate model which assumes C2v instead of the actual C2 site symmetry were diagonalized. Excellent correlations were obtained between experimental transition energies and the computed level structures. We also report the results of previously unpublished experimental spectroscopic investigations of Nd3+ and Sm3+:LaF3, as well as predicted energy levels for Pm3+:LaF3. The spectroscopic data for each ion were independently interpreted using an effective‐operator model, then the model parameters were intercompared. Systematic trends have been identified, and a comprehensive energy level diagram is presented.
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