High-Tc superconductivity has recently been discovered in Ruddlesden-Popper phase nickelates under pressure, where the low-energy electronic structure is dominated by Ni dx2−y2 and dz2 orbitals. However, the respective roles of these orbitals in superconductivity remain unclear. Here, by combining X-ray absorption, electron energy loss spectroscopy, and density functional theory calculations on La4Ni3O10 single crystals, we identify ligand holes in the px,y orbitals of planar oxygen and the pz orbitals of apical oxygen, which hybridize with the Ni dx2−y2 and dz2 orbitals, respectively. These ligand holes enable orbital-selective O K-edge resonant inelastic X-ray scattering (RIXS) study, which reveals that dx2−y2 states dominate the low-energy charge excitations and are more itinerant. We also observe a ∼0.1 eV bimagnon through RIXS and Raman spectroscopy, which leads to an interlayer superexchange interaction Jz of ∼50 meV. Our results reveal distinct contributions of Ni dx2−y2 and dz2 orbitals to the electronic and magnetic structure and provide direct experimental insights to understand the RP-phase nickelate superconductors.
@article{arxiv.2509.20727,
title = {Distinct orbital contributions to electronic and magnetic structures in La$_{4}$Ni$_{3}$O$_{10}$},
author = {Shilong Zhang and Hengyuang Zhang and Zehao Dong and Jie Li and Qian Xiao and Mengwu Huo and Hsiao-Yu Huang and Di-Jing Huang and Yayu Wang and Yi Lu and Zhen Chen and Meng Wang and Yingying Peng},
journal= {arXiv preprint arXiv:2509.20727},
year = {2026}
}