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We discuss recent progress and future prospects for the analysis of the 4fN–15d excited states of lanthanide ions in host materials. We demonstrate how ab initio calculations for Ce3+ in LiYF4 may be used to estimate crystal‐field and spin‐orbit parameters for the 4f1 and 5d1 configurations. We show how excited‐state absorption may be used to probe the electronic and geometric structure of the 4fN...
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