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High-resolution photoemission spectroscopy and realistic ab-initiocalculations have been employed to analyze the onset and progression of d-sphybridization in Fe impurities deposited on alkali metal films. The interplaybetween delocalization, mediated by the free-electron environment, and Coulombinteraction among d-electrons gives rise to complex electronic configurations.The multiplet structure of a single Fe atom evolves and gradually dissolvesinto a quasiparticle peak near the Fermi level with increasing the hostelectron density. The effective multi-orbital impurity problem within the exactdiagonalization scheme describes the whole range of hybridizations.

Correlated Electrons Step-by-Step: Itinerant-to-Localized Transition of Fe Impurities in Free-Electron Metal Hosts