21 March, 2025Electronic structure origins of anomalous magnetic character in the ferromagnetic trilayer Sr4Ru3O10 are investigated using angle- and spin-resolved photoemission. The authors highlight two momentum-separated narrow spectral peaks 30 𝑚𝑒𝑉 below the Fermi-level with opposite-spin polarization as well as dramatic temperature-dependent coherence-incoherence crossover behavior. In addition, comparison to spin-polarized band theory reveals that they possess different antibonding versus nonbonding 𝑑𝑥𝑧/𝑦𝑧 orbital character, and thus different spatial localization in the central versus outer layers, with implications for its in-plane metamagnetic behavior.