Orbital and Spin Character of Doped Carriers in Infinite-Layer Nickelates

Abstract

The recent discovery of superconductivity in Nd${}_{1-x}$Sr${}_x$NiO${}_2$ has drawn significant attention in the field. A key open question regards the evolution of the electronic structure with respect to hole doping. Here, we exploit x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) to probe the doping dependent electronic structure of the NiO${}_2$ planes. Upon doping, a higher energy feature in Ni $L_3$ edge XAS develops in addition to the main absorption peak. By comparing our data to atomic multiplet calculations including $D_{4h}$ crystal field, the doping induced feature is consistent with a $d^8$ spin singlet state, in which doped holes reside in the $d_{x^2-y^2}$ orbitals, similar to doped single band Hubbard models. This is further supported by orbital excitations observed in RIXS spectra, which soften upon doping, corroborating with Fermi level shift associated with increasing holes in the $d_{x^2-y^2}$ orbital.

6 pages, 4 figures. Supplemental material included

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• Superconductivity in PrNiO2 infinite-layer nickelates
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• Role of Oxygen States in the Low Valence Nickelate La${}_4$Ni${}_3$O${}_8$
• Microscopic Theory of Superconducting Phase Diagram in Infinite-Layer Nickelates
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• Screening in a two-band model for superconducting infinite-layer nickelate
• Superconductivity in the parent infinite-layer nickelate NdNiO${}_2$
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• Topotactically induced oxygen vacancy order in nickelate single crystals
• Investigation of spin excitations and charge order in bulk crystals of the infinite-layer nickelate LaNiO${}_2$
• Photo-induced charge-transfer renormalization in NiO
• Comparative study of charge order in undoped infinite-layer nickelate superconductors
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• Charge order and superconductivity in a minimal two-band model for infinite-layer nickelates
• Emergent electronic landscapes in a novel valence-ordered nickelate with tri-component nickel coordination
• Two Distinct Charge Orders in Infinite-layer PrNiO2+δ revealed by Resonant X-ray Diffraction
• Unraveling p-type and n-type interfaces in Superconducting Infinite-Layer Nickelate thin films
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• Signatures of canted antiferromagnetism in infinite-layer nickelates studied by x-ray magnetic dichroism
• The emergence of antiferromagnetic correlations and Kondo-like features in a two-band model for infinite-layer nickelates
• Softening of $dd$ excitation in the resonant inelastic x-ray scattering spectra as a signature of Hund's coupling in nickelates
• Capping effects on spin and charge excitations in parent and superconducting Nd1-xSrxNiO2
• A Broken Translational Symmetry State in an Infinite-Layer Nickelate
• Resonant inelastic x-ray scattering data for Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates
• Absence of mixed valency for Pr in pristine and hole-doped PrNiO${}_2$
• Magnetic excitations in Nd${}_{n+1}$Ni${}_n$O${}_{3n+1}$ Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering
• On the nature of valence charge and spin excitations via multi-orbital Hubbard models for infinite-layer nickelates
• Superconducting phase diagram of multi-layer square-planar nickelates
• Character of Doped Holes in Nd${}_{1-x}$Sr${}_x$NiO${}_2$