Abstract

We use Ru L3L_3-edge resonant inelastic x-ray scattering (RIXS) to study the full range of excitations in Ca3_3Ru2_2O7_7 from meV-scale magnetic dynamics through to the eV-scale interband transitions. This bilayer 4d4d-electron correlated metal expresses a rich phase diagram, displaying long range magnetic order below 56 K followed by a concomitant structural, magnetic and electronic transition at 48 K. In the low temperature phase we observe a magnetic excitation with a bandwidth of ∼\sim30 meV and a gap of ∼\sim8 meV at the zone center, in excellent agreement with inelastic neutron scattering data. The dispersion can be modeled using a Heisenberg Hamiltonian for a bilayer S=1\mathrm{S}=1 system with single ion anisotropy terms. At a higher energy loss, dddd-type excitations show heavy damping in the presence of itinerant electrons, giving rise to a fluorescence-like signal appearing between the t2gt_{2g} and ege_g bands. At the same time, we observe a resonance originating from localized t2gt_{2g} excitations, in analogy to the structurally related Mott-insulator Ca2_2RuO4_4. But whereas Ca2_2RuO4_4 shows sharp separate spin-orbit excitations and Hund's-rule driven spin-state transitions, here we identify only a single broad asymmetric feature. These results indicate that local intra-ionic interactions underlie the correlated physics in Ca3_3Ru2_2O7_7, even as the excitations become strongly mixed in the presence of itinerant electrons.

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