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Resonant inelastic x-ray scattering is used to investigate the electronicorigin of orbital polarization in nickelate heterostructures taking$\mathrm{LaTiO_3-LaNiO_3-3x(LaAlO_3)}$, a system with exceptionally largepolarization, as a model system. We find that heterostructuring generates onlyminor changes in the Ni $3d$ orbital energy levels, contradicting theoften-invoked picture in which changes in orbital energy levels generateorbital polarization. Instead, O $K$-edge x-ray absorption spectroscopydemonstrates that orbital polarization is caused by an anisotropicreconstruction of the oxygen ligand hole states. This provides an explanationfor the limited success of theoretical predictions based on tuning orbitalenergy levels and implies that future theories should focus on anisotropichybridization as the most effective means to drive large changes in electronicstructure and realize novel emergent phenomena.

Orbital engineering in nickelate heterostructures driven by anisotropic oxygen hybridization rather than orbital energy levels