Ground state oxygen holes and the metal-insulator transition in the negative charge transfer rare-earth nickelates

Abstract

The metal-insulator transitions and the intriguing physical properties of rare-earth perovskite nickelates have attracted considerable attention in recent years. Nonetheless, a complete understanding of these materials remains elusive. Here, taking a NdNiO3 thin film as a representative example, we utilize a combination of x-ray absorption and resonant inelastic x-ray scattering (RIXS) spectroscopies to resolve important aspects of the complex electronic structure of the rare-earth nickelates. The unusual coexistence of bound and continuum excitations observed in the RIXS spectra provides strong evidence for the abundance of oxygen 2p holes in the ground state of these materials. Using cluster calculations and Anderson impurity model interpretation, we show that these distinct spectral signatures arise from a Ni 3d8 configuration along with holes in the oxygen 2p valence band, confirming suggestions that these materials do not obey a conventional positive charge-transfer picture, but instead exhibit a negative charge-transfer energy, in line with recent models interpreting the metal to insulator transition in terms of bond disproportionation.

arXiv comment27 pages, 6 figures

References in corpus (25)

• Resonant Inelastic X-ray Scattering Studies of Elementary Excitations
• Orbital order and possible superconductivity in LaNiO3/LaMO3 superlattices
• Metal-insulator transition in ultrathin LaNiO3 films
• Site-selective Mott transition in rare earth nickelates
• Charge disproportionation without charge transfer in the rare-earth nickelates as a possible mechanism for the metal-insulator transition
• Orbital reflectometry
• Heterointerface engineered electronic and magnetic phases of NdNiO3 thin films
• Spin and charge ordering in self-doped Mott insulators
• Origins of bad metal conductivity and the insulator-metal transition in the rare-earth nickelates
• Asymmetric orbital-lattice interactions in ultra-thin correlated oxide films
• Ultrafast strain engineering in complex oxide heterostructures
• Role of magnetic and orbital ordering at the metal-insulator transition in NdNiO3
• Low-energy description of the metal-insulator transition in the rare-earth nickelates
• Strain and composition dependence of the orbital polarization in nickelate superlattices
• Theory of the magnetic and metal-insulator transitions in RNiO3 bulk and layered structures
• Electronic Transitions in Strained SmNiO_3 Thin Films
• Tailoring the electronic transitions of NdNiO_3 films through (111)_pc oriented interfaces
• Localized vs. delocalized character of charge carriers in LaAlO3/ SrTiO3 superlattices
• Evidence for mass renormalization in LaNiO$"" sub 3_: an in situ soft x-ray photoemission study of epitaxial films
• Tuning the metal-insulator transition in NdNiO3 heterostructures via Fermi surface instability and spin-fluctuations
• Metal-insulator transition and orbital reconstruction in Mott quantum wells of NdNiO${}_3$
• Key role of lattice symmetry in the metal-insulator transition of NdNiO3 films
• Orbital engineering in nickelate heterostructures driven by anisotropic oxygen hybridization rather than orbital energy levels
• Unusual valence, negative charge-transfer gaps and self-doping in transition-metal compounds
• Ordering and criticality in an underscreened Kondo chain

Cited by in corpus (103)

• Electronic structure of the parent compound of superconducting infinite-layer nickelates
• Visualization of Oxygen Vacancies and Self-doped Ligand Holes in La3Ni2O7-δ
• Electronic correlations and superconducting instability in La${}_3$Ni${}_2$O${}_7$ under high pressure
• Charge-spin correlation in van der Waals antiferromagenet NiPS3
• Interlayer Coupling Driven High-Temperature Superconductivity in La${}_3$Ni${}_2$O${}_7$ Under Pressure
• Doping evolution of the Mott-Hubbard landscape in infinite-layer nickelates
• Structurally Triggered Metal-Insulator Transition in Rare-Earth Nickelates
• Bond disproportionation and dynamical charge fluctuations in the perovskite rare earth nickelates
• Electronic and magnetic excitations in La${}_3$Ni${}_2$O${}_7$
• Hexagonal Perovskites as Quantum Materials
• Orbital and Spin Character of Doped Carriers in Infinite-Layer Nickelates
• Electronic Structure Trends Across the Rare-Earth Series in Superconducting Infinite Layer Nickelates
• Observation of perfect diamagnetism and interfacial effect on the electronic structures in Nd0.8Sr0.2NiO2 superconducting infinite layers
• Quantum anomalous Hall effect from inverted charge transfer gap
• Absence of $3a_0$ Charge Density Wave Order in the Infinite Layer Nickelates
• LDA+DMFT approach to resonant inelastic x-ray scattering in correlated materials
• Mott Transition and Magnetism in Rare Earth Nickelates and its Fingerprint on the X-ray Scattering
• Complex magnetic order in nickelate slabs
• Tunable resistivity exponents in the metallic phase of epitaxial nickelates
• Electronic structure of superconducting nickelates probed by resonant photoemission spectroscopy
• Unexpected 3+ valence of iron in FeO${}_2$, a geologically important material lying "in between" oxides and peroxides
• Anti-doping in Insulators and Semiconductors having Intermediate Bands with Trapped Carriers
• Doping Dependence of Collective Spin and Orbital Excitations in Spin 1 Quantum Antiferromagnet La${}_{2-x}$Sr${}_x$NiO${}_4$ Observed by X-rays
• Reproducibility and off-stoichiometry issues in nickelate thin films grown by pulsed laser deposition
• Strain-Driven Disproportionation at a Correlated Oxide Metal-Insulator Transition
• Fingerprints of an Exotic Orbital-Selective Mott Phase in the Block Magnetic State of BaFe${}_2$Se${}_3$ Ladders
• Quantum Monte Carlo study of lattice polarons in the two-dimensional multi-orbital Su-Schrieffer-Heeger model
• Exploring Quantum Materials with Resonant Inelastic X-Ray Scattering
• Crossover from Collective to Incoherent Spin Excitations in Superconducting Cuprates Probed by Detuned Resonant Inelastic X-ray Scattering
• Renormalization of effective interactions in a negative charge-transfer insulator
• Site-selective Probe of Magnetic Excitations in Rare-earth Nickelates using Resonant Inelastic X-ray Scattering
• Continuum Charge Excitations in High-Valence Transition-Metal Oxides Revealed by Resonant Inelastic X-ray Scattering
• LiNiO${}_2$ as a high-entropy charge- and bond-disproportionated glass
• High-density electron doping of SmNiO${}_3$ from first principles
• Distortion mode anomalies in bulk PrNiO${}_3$ illustrating the potential of symmetry-adapted distortion mode analysis for the study of phase transitions
• Disentangled cooperative orderings in artificial rare-earth nickelates
• Soft X-ray Spectroscopy of Low-Valence Nickelates
• Synthesis and electronic properties of Nd${}_{n+1}$Ni${}_n$O${}_{3n+1}$ Ruddlesden-Popper nickelate thin films
• Hybridization-switching induced Mott transition in ABO${}_3$ perovskites
• Observation of an antiferromagnetic quantum critical point in high-purity LaNiO${}_3$
• Sudden collapse of magnetic order in oxygen deficient nickelate films
• Tuning spin excitations in magnetic films by confinement
• Core-level x-ray photoemission and Raman spectroscopy studies on electronic structures in Mott-Hubbard type nickelate oxide NdNiO${}_2$
• Epitaxial engineering of flat silver fluorides cuprate analogs
• Superconductivity in PrNiO2 infinite-layer nickelates
• Anisotropic character of the metal-to-metal transition in Pr4Ni${}_3$O${}_{10}$
• Orbital dynamics during an ultrafast insulator to metal transition
• Anomalous electron transport in epitaxial NdNiO${}_3$ films
• X-ray spectroscopy of rare-earth nickelate LuNiO${}_3$: LDA+DMFT study
• Electronic Localization in CaVO3 Films via Bandwidth Control
• The Valence Transition Model of Pseudogap, Charge-Order and Superconductivity in Electron- and Hole-Doped Copper Oxides
• First-principles study of electron and hole doping in perovskite nickelates
• A fundamental correlative spectroscopic study on LixNiO2 and NaNiO2
• Evolution of the SrTiO${}_3$ surface electronic state as a function of LaAlO${}_3$ overlayer thickness
• Epitaxial strain modulated electronic properties of interface controlled nickelate superlattice
• Spectroscopic comprehension of Mott-Hubbard insulator to negative charge transfer metal transition in LaNi_{x}V_{1-x}O_{3} thin films
• High pO2 Floating Zone Crystal Growth of the Perovskite Nickelate PrNiO3
• Resolving the nature of electronic excitations in resonant inelastic x-ray scattering
• Superconductivity in a layered cobalt oxychalcogenide Na${}_2$CoSe${}_2$O with a triangular lattice
• Hybridization driving distortions and multiferroicity in rare-earth nickelates
• Electronic structure of Pr2MnNiO6 from x-ray photoemission, absorption and density functional theory
• Control of the metal-insulator transition in NdNiO${}_3$ thin films through the interplay between structural and electronic properties
• Anisotropic magnetic excitations and incipient Néel order in Ba(Fe${}_{1-x}$Mn${}_x$)${}_2$As${}_2$
• Resonant inelastic x-ray scattering study of bond order and spin excitations in nickelate thin-film structures
• Assessing the correlated electronic structure of lanthanum nickelates
• Metal-insulator transition and local-moment collapse in negative charge-transfer CaFeO${}_3$ under pressure
• Conductivity noise across temperature driven transitions of rare-earth nickelate heterostructures
• Negative charge transfer energy in correlated compounds
• Emergent c-axis magnetic helix in manganite-nickelate superlattices
• Spin and charge excitations in the correlated multiband metal Ca3Ru2O7
• Probing photo-induced rearrangements in the NdNiO${}_3$ magnetic spiral with polarization-sensitive ultrafast resonant soft x-ray scattering
• Emergent electronic landscapes in a novel valence-ordered nickelate with tri-component nickel coordination
• FeS2 monolayer: a high valence and high-$T_{\mathrm{C}}$ Ising ferromagnet
• Intertwined charge and spin instability of La${}_3$Ni${}_2$O${}_7$
• Finite-temperature phase diagram of (111) nickelate bilayers
• Spin waves and orbital contribution to ferromagnetism in a topological metal
• Dispersionless orbital excitations in (Li,Fe)OHFeSe superconductors
• PERSPECTIVE: Emergent phases in rare earth nickelate heterostructures
• Effects of reduced dimensionality, crystal field, electron-lattice coupling, and strain on the ground-state of a rare-earth nickelates monolayer
• Interplay between electron correlations, magnetic state, and structural confinement in LaNiO3 ultrathin films
• Unusual coexistence of negative/positive charge-transfer in mixed-valence Na${}_x$Ca${}_{1-x}$Cr${}_2$O${}_4$
• Ferromagnetic Negative Charge-Transfer Insulator: from Theoretical Proposal to Material Realization
• Phenomenological Three-Orbital Spin-Fermion Model for Cuprates
• Magnetic excitations in Nd${}_{n+1}$Ni${}_n$O${}_{3n+1}$ Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering
• Cooling a polaronic liquid: Phase mixture and pseudogap-like spectra in superconducting $B{a}_{1-x}{K}_{x}Bi{O}_3$
• Spin-orbital liquid in Ba${}_3$CuSb${}_2$O${}_9$ stabilized by oxygen holes
• Time-resolved photoemission and RIXS study of a site-selective Mott insulator
• Temperature-Dependent Dynamic Disproportionation in LiNiO${}_2$
• Persistence of small polarons into the superconducting phase of Ba${}_{1-x}$K${}_x$BiO${}_3$
• High-resolution valence band RIXS at the actinide M${}_{4,5}$-edges
• Valence Transition Theory of the Pressure-Induced Dimensionality Crossover in Superconducting Sr${}_{14-x}$Ca${}_x$Cu${}_{24}$O${}_{41}$
• Grotthuss-type oxygen hole polaron transport in desodiated Na${}_2$Mn${}_3$O${}_7$
• Weak electronic correlations in the cobalt oxychalcogenide superconductor Na2CoSe2O
• Signatures of polarized chiral spin disproportionation in rare earth nickelates
• Emergence and tunability of Fermi-pocket and electronic instabilities in layered Nickelates
• Emergence of interfacial magnetism in strongly-correlated nickelate-titanate superlattices
• Enhanced Itinerant Ferromagnetism in Hole-doped Transition Metal Oxides: Beyond the Canonical Double Exchange Mechanism
• Valency, charge-transfer, and orbital-dependent correlation in bilayer nickelates Nd3Ni2O7
• Revisiting the metal-to-metal transition in $2H$-AgNiO${}_2$
• High resolution resonant inelastic EUV scattering from orbital excitations in a Heisenberg antiferromagnet
• Metal-insulator transition in CaCu${}_3$Fe${}_4$O${}_{12}$
• Probing electronic and magnetic transitions of short periodic nickelate superlattices using synchrotron x-ray
• Charge disproportionation and nano phase separation in $R$SrNiO${}_4$