Distinct orbital contributions to electronic and magnetic structures in La${}_4$Ni${}_3$O${}_{10}$

Abstract

High-T${}_c$ superconductivity has recently been discovered in Ruddlesden-Popper phase nickelates under pressure, where the low-energy electronic structure is dominated by Ni $d_{x^2-y^2}$ and $d_{z^2}$ 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 La${}_4$Ni${}_3$O${}_{10}$ single crystals, we identify ligand holes in the $p_{x,y}$ orbitals of planar oxygen and the $p_z$ orbitals of apical oxygen, which hybridize with the Ni $d_{x^2-y^2}$ and $d_{z^2}$ orbitals, respectively. These ligand holes enable orbital-selective O K-edge resonant inelastic X-ray scattering (RIXS) study, which reveals that $d_{x^2-y^2}$ states dominate the low-energy charge excitations and are more itinerant. We also observe a $\sim$0.1 eV bimagnon through RIXS and Raman spectroscopy, which leads to an interlayer superexchange interaction J${}_z$ of $\sim$50 meV. Our results reveal distinct contributions of Ni $d_{x^2-y^2}$ and $d_{z^2}$ orbitals to the electronic and magnetic structure and provide direct experimental insights to understand the RP-phase nickelate superconductors.

References in corpus (35)

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• Superconductivity in pressurized trilayer La${}_4$Ni${}_3$O${}_{10-\delta }$ single crystals
• Visualization of Oxygen Vacancies and Self-doped Ligand Holes in La3Ni2O7-δ
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• Correlated electronic structure of La${}_3$Ni${}_2$O${}_7$ under pressure
• Orbital-Dependent Electron Correlation in Double-Layer Nickelate La3Ni2O7
• Bilayer $t$-$J$-$J_{\perp }$ Model and Magnetically Mediated Pairing in the Pressurized Nickelate La${}_3$Ni${}_2$O${}_7$
• Evidence for charge and spin order in single crystals of La${}_3$Ni${}_2$O${}_7$ and La${}_3$Ni${}_2$O${}_6$
• Electronic structure, dimer physics, orbital-selective behavior, and magnetic tendencies in the bilayer nickelate superconductor La${}_3$Ni${}_2$O${}_7$ under pressure
• Ambient-pressure superconductivity onset above 40 K in bilayer nickelate ultrathin films
• Pressure-induced superconductivity in polycrystalline La3Ni2O7
• Structural phase transition, $s_{\pm }$-wave pairing and magnetic stripe order in the bilayered nickelate superconductor La${}_3$Ni${}_2$O${}_7$ under pressure
• Signature of superconductivity in pressurized La${}_4$Ni${}_3$O${}_{10}$
• Character of the "normal state" of the nickelate superconductors
• Electronic and magnetic excitations in La${}_3$Ni${}_2$O${}_7$
• High-$T_c$ superconductivity by mobilizing local spin singlets and possible route to higher $T_c$ in pressurized La${}_3$Ni${}_2$O${}_7$
• High-T${}_C$ superconductivity in $\mathrm{L}{\mathrm{a}}_3\mathrm{N}{\mathrm{i}}_2{\mathrm{O}}_7$ based on the bilayer two-orbital t-J model
• Neutron Scattering Studies on the High-$T_c$ Superconductor La${}_3$Ni${}_2$O${}_{7-\delta }$ at Ambient Pressure
• Structural transition, electric transport, and electronic structures in the compressed trilayer nickelate La4Ni3O10
• Quenched pair breaking by interlayer correlations as a key to superconductivity in La${}_3$Ni${}_2$O${}_7$
• Multiband Metallic Ground State in Multilayered Nickelates La${}_3$Ni${}_2$O${}_7$ and La${}_4$Ni${}_3$O${}_{10}$ Probed by ${}^{139}$La-NMR at Ambient Pressure
• Effective model and $s_{\pm }$-wave superconductivity in trilayer nickelate La${}_4$Ni${}_3$O${}_{10}$
• Trilayer multi-orbital models of $\mathrm{L}{\mathrm{a}}_4\mathrm{N}{\mathrm{i}}_3{\mathrm{O}}_{10}$
• Orbital-selective Superconductivity in the Pressurized Bilayer Nickelate La${}_3$Ni${}_2$O${}_7$: An Infinite Projected Entangled-Pair State Study
• Density-wave-like gap evolution in La${}_3$Ni${}_2$O${}_7$ under high pressure revealed by ultrafast optical spectroscopy
• Signature of Superconductivity in Pressurized Trilayer-nickelate Pr${}_4$Ni${}_3$O${}_{10-\delta }$
• The $s^{\pm }$-Wave Superconductivity in the Pressurized La${}_4$Ni${}_3$O${}_{10}$
• Pressure-induced superconductivity in La${}_4$Ni${}_3$O${}_{10+\delta }$ ($\delta$ = 0.04 and -0.01)
• Interlayer Pairing Induced Partially Gapped Fermi Surface in Trilayer La${}_4$Ni${}_3$O${}_{10}$ Superconductors
• Interstitial oxygen order and its competition with superconductivity in La${}_2$PrNi${}_2$O${}_{7+\delta }$
• Superconductivity in the parent infinite-layer nickelate NdNiO${}_2$
• Superconductivity in La${}_4$Ni${}_3$O${}_{10}$ Under Pressure
• Softening of $dd$ excitation in the resonant inelastic x-ray scattering spectra as a signature of Hund's coupling in nickelates
• Magnetic excitations in Nd${}_{n+1}$Ni${}_n$O${}_{3n+1}$ Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering