Magnetic correlations in infinite-layer nickelates: an experimental and theoretical multi-method study

Abstract

We report a comprehensive study of magnetic correlations in LaNiO${}_2$, a parent compound of the recently discovered family of infinite-layer (IL) nickelate superconductors, using multiple experimental and theoretical methods. Our specific heat, muon-spin rotation ($\mu$SR), and magnetic susceptibility measurements on polycrystalline LaNiO${}_2$ show that long-range magnetic order remains absent down to 2 K. Nevertheless, we detect residual entropy in the low-temperature specific heat, which is compatible with a model fit that includes paramagnon excitations. The $\mu$SR and low-field static and dynamic magnetic susceptibility measurements indicate the presence of short-range magnetic correlations and glassy spin dynamics, which we attribute to local oxygen non-stoichiometry in the average infinite-layer crystal structure. This glassy behavior can be suppressed in strong external fields, allowing us to extract the intrinsic paramagnetic susceptibility. Remarkably, we find that the intrinsic susceptibility shows non-Curie-Weiss behavior at high temperatures, in analogy to doped cuprates that possess robust non-local spin fluctuations. The distinct temperature dependence of the intrinsic susceptibility of LaNiO${}_2$ can be theoretically understood by a multi-method study of the single-band Hubbard model in which we apply complementary cutting-edge quantum many-body techniques (dynamical mean-field theory, cellular dynamical mean-field theory and the dynamical vertex approximation) to investigate the influence of both short- and long-ranged correlations. Our results suggest a profound analogy between the magnetic correlations in parent (undoped) IL nickelates and doped cuprates.

arXiv comment18 pages, 14 figures

References in corpus (95)

• Continuous-time Monte Carlo methods for quantum impurity models
• A Common Thread: the pairing interaction for the unconventional superconductors
• Quantum Cluster Theories
• Continuous Time Quantum Monte Carlo method for fermions
• musrfit: A free platform-independent framework for muSR data analysis
• The Hubbard Model
• TRIQS: A Toolbox for Research on Interacting Quantum Systems
• Solutions of the Two Dimensional Hubbard Model: Benchmarks and Results from a Wide Range of Numerical Algorithms
• Intense paramagnon excitations in a large family of high-temperature superconductors
• Diagrammatic routes to nonlocal correlations beyond dynamical mean field theory
• High Temperature Superconductivity in Iron Pnictides and Chalcogenides
• The Hubbard model: A computational perspective
• Dynamical vertex approximation - a step beyond dynamical mean field theory
• Superconducting Dome in Nd${}_{1-x}$Sr${}_x$NiO${}_2$ Infinite Layer Films
• Electronic structure of the parent compound of superconducting infinite-layer nickelates
• Phase diagram and superconducting dome of infinite-layer $\mathrm{N}{\mathrm{d}}_{1-\mathrm{x}}\mathrm{S}{\mathrm{r}}_{\mathrm{x}}\mathrm{Ni}{\mathrm{O}}_2$ thin films
• Infinite Layer LaNiO(2): Ni(1+)is not Cu(2+)
• A superconducting praseodymium nickelate with infinite layer structure
• Nickelate superconductivity without rare-earth magnetism: (La,Sr)NiO${}_2$
• Persistence of magnetic excitations in La2-xSrxCuO4 from the undoped insulator to the heavily overdoped non-superconducting metal
• Plaquette Ordered Phase and Quantum Phase Diagram in the Spin-1/2 J1-J2 Square Heisenberg Model
• Signatures of Spin Glass Freezing in NiO Nanoparticles
• Formation of 2D single-component correlated electron system and band engineering in the nickelate superconductor NdNiO2
• Self-doped Mott insulator for parent compounds of nickelate superconductors
• The critical nature of the Ni spin state in doped NdNiO${}_2$
• Similarities and differences between infinite-layer nickelates and cuprates and implications for superconductivity
• Robust $d_{x^2-y^2}$-wave superconductivity of infinite-layer nickelates
• Model construction and a possibility of cuprate-like pairing in a new d9 nickelate superconductor (Nd,Sr)NiO2
• Nickelate superconductors -- a renaissance of the one-band Hubbard model
• Doping evolution of the Mott-Hubbard landscape in infinite-layer nickelates
• Fate of the false Mott-Hubbard transition in two dimensions
• Tracking the Footprints of Spin Fluctuations: A MultiMethod, MultiMessenger Study of the Two-Dimensional Hubbard Model
• Magnetic neutron scattering in hole doped cuprate superconductors
• Nickelate superconductors $--$ Multiorbital nature and spin freezing
• High pressure sequence of Ba_3NiSb_2O_9 structural phases: new $S=1$ quantum spin-liquids based on Ni^{2+}
• Topotactic hydrogen in nickelate superconductors and akin infinite-layer oxides ABO2
• New valence bond crystal phase of a frustrated spin-1/2 square lattice antiferromagnet
• Comparing pertinent effects of antiferromagnetic fluctuations in the two and three dimensional Hubbard model
• Many-body Electronic Structure of NdNiO${}_2$ and CaCuO${}_2$
• Fluctuation diagnostics of the electron self-energy: Origin of the pseudogap physics
• A substantial hybridization between correlated Ni-d orbital and itinerant electrons in infinite-layer nickelates
• Pseudogap and antiferromagnetic correlations in the Hubbard model
• Synthesis and characterization of bulk Nd1-xSrxNiO2 and Nd1-xSrxNiO3
• Influence of apical oxygen on the extent of in-plane exchange interaction in cuprate superconductors
• Hund's metal physics: from SrNiO${}_2$ to NdNiO${}_2$
• Mott insulating states with competing orders in the triangular lattice Hubbard model
• Critical properties of the half-filled Hubbard model in three dimensions
• Induced magnetic two-dimensionality by hole doping in the superconducting infinite-layer nickelate Nd${}_{1-x}$Sr${}_x$NiO${}_2$
• Dispersive spin excitations in highly overdoped cuprates revealed by resonant inelastic x-ray scattering
• Charge Segregation, Cluster Spin-Glass and Superconductivity in La1.94Sr0.06CuO4
• Orbital and Spin Character of Doped Carriers in Infinite-Layer Nickelates
• The new versatile general purpose surface-muon instrument (GPS) based on silicon photomultipliers for $\mu$SR measurements on a continuous-wave beam
• Fermi surfaces, electron-hole asymmetry and correlation kink in a three-dimensional Fermi liquid LaNiO${}_3$
• Multiorbital processes rule the Nd${}_{1-x}$Sr${}_x$NiO${}_2$ normal state
• Continuous Time Quantum Monte Carlo Method for Fermions: Beyond Auxiliary Field Framework
• Lifshitz transition and frustration of magnetic moments in infinite-layer NdNiO${}_2$ upon hole-doping
• Type II $t-J$ model in superconducting nickelate Nd${}_{1-x}$Sr${}_x$NiO${}_2$
• Electronic Structure Trends Across the Rare-Earth Series in Superconducting Infinite Layer Nickelates
• Isotropic Pauli-Limited Superconductivity in the Infinite Layer Nickelate Nd${}_{0.775}$Sr${}_{0.225}$NiO${}_2$
• Ab initio dynamical vertex approximation
• Effective Hamiltonian for superconducting Ni oxides Nd${}_{1-x}$Sr${}_x$NiO${}_2$
• Electronic and Magnetic Structure of Infinite-layer ${\text{NdNiO}}_2$: Trace of Antiferromagnetic Metal
• Topotactic transformation of single-crystals: from perovskite to infinite-layer nickelates
• Strong Superexchange in a $d^{9-\delta }$ Nickelate Revealed by Resonant Inelastic X-Ray Scattering
• Stripes, Antiferromagnetism, and the Pseudogap in the Doped Hubbard Model at Finite Temperature
• $f$-electron and magnetic ordering effects in nickelates LaNiO${}_2$ and NdNiO${}_2$: remarkable role of the cuprate-like $3d_{x^2-y^2}$ band
• Why the critical temperature of high-$T_{\mathrm{c}}$ cuprate superconductors is so low: The importance of the dynamical vertex structure
• Fluctuation-frustrated flat band instabilities in NdNiO2
• Spin and charge correlations across the metal-to-insulator crossover in the half-filled $2d$ Hubbard model
• Quantum criticality with a twist - interplay of correlations and Kohn anomalies in three dimensions
• Electronic structure and magnetism in infinite-layer nickelates RNiO${}_2$ (R= La-Lu)
• NMR Evidence of Antiferromagnetic Spin Fluctuations in Nd${}_{0.85}$Sr${}_{0.15}$NiO${}_2$
• Nickelate superconductors: an ongoing dialog between theory and experiments
• Enhanced thermal Hall effect in the square-lattice Néel state
• Randomness-induced quantum spin liquid behavior in the $s=\frac{1}{2}$ random $J_1$-$J_2$ Heisenberg antiferromagnet on the square lattice
• Universal spin-glass behaviour in bulk LaNiO2, PrNiO2 and NdNiO2
• Electronic correlations and magnetic interactions in infinite-layer NdNiO${}_2$
• Dynamical vertex approximation for the two-dimensional Hubbard model
• Dependence of DFT+DMFT Results on the Construction of the Correlated Orbitals
• Probing exotic spin correlations by Muon Spin depolarization measurements with applications to spin glass dynamics
• Intrinsic Spin Susceptibility and Pseudogap-like Behavior in Infinite-Layer LaNiO2
• On the separability of dynamical and non-local correlations in three dimensions
• Knight shifts, nuclear spin-relaxation rates, and spin echo decay times in the pseudogap regime of the cuprates: Simulation and relation to experiment
• Quantum criticality in the two-dimensional periodic Anderson model
• Short-range magnetic interactions and spin-glass behavior in the quasi-2D nickelate Pr4Ni3O8
• How to read between the lines of electronic spectra: the diagnostics of fluctuations in strongly correlated electron systems
• Soft X-ray Spectroscopy of Low-Valence Nickelates
• Real-space cluster dynamical mean-field theory: Center focused extrapolation on the one- and two particle level
• Hund-Heisenberg model in superconducting infinite-layer nickelates
• Magnetic properties and pseudogap formation in infinite-layer nickelates: insights from the single-band Hubbard model
• Spin excitations in nickelate superconductors
• Charge-stripe order, antiferromagnetism, and spin dynamics in the cuprate-analog nickelate La${}_4$Ni${}_3$O${}_8$
• Anisotropy of electronic correlations: On the applicability of local theories to layered materials
• Ferromagnetic spin correlations in the two-dimensional Hubbard model
• Magnetic excitations in infinite-layer nickelates

Cited by in corpus (29)

• Intrinsic magnetism in superconducting infinite-layer nickelates
• Synthesis and physical properties of LaNiO${}_2$ crystals
• Magnetic properties and pseudogap formation in infinite-layer nickelates: insights from the single-band Hubbard model
• Investigation of hydrogen incorporations in bulk infinite-layer nickelates
• Microscopic Theory of Superconducting Phase Diagram in Infinite-Layer Nickelates
• On the origin of topotactic reduction effect for superconductivity in infinite-layer nickelates
• Topotactic-hydrogen forms chains in $AB$O${}_2$ nickelate superconductors
• Phase formation in hole- and electron-doped rare-earth nickelate single crystals
• Mott transition and pseudogap of the square-lattice Hubbard model: results from center-focused cellular dynamical mean-field theory
• Large upper critical fields and dimensionality crossover of superconductivity in infinite-layer nickelate La${}_{0.8}$Sr${}_{0.2}$NiO${}_2$
• Antiferromagnetic fluctuations and a dominant $d_{xy}$-wave pairing symmetry in nickelate-based superconductors
• Correlation-temperature phase diagram of prototypical infinite layer rare earth nickelates
• Distinct electridelike nature of infinite-layer nickelates and the resulting theoretical challenges to calculate their electronic structure
• Stabilization of singlet hole-doped state in infinite-layer nickelate superconductors
• Scanning SQUID study of ferromagnetism and superconductivity in infinite-layer nickelates
• Investigation of spin excitations and charge order in bulk crystals of the infinite-layer nickelate LaNiO${}_2$
• Magnetism in doped infinite-layer NdNiO2 studied by combined density functional theory and dynamical mean-field theory
• Possible structural quantum criticality tuned by rare-earth ion substitution in infinite-layer nickelates
• Low-energy plasmon excitations in infinite-layer nickelates
• Magnetism-Enhanced Strong Electron-Phonon Coupling in Infinite-Layer Nickelate
• Signatures of canted antiferromagnetism in infinite-layer nickelates studied by x-ray magnetic dichroism
• Influence of $f$ Electrons on the Electronic Band Structure of Rare-Earth Nickelates
• Electronic correlations and spin-charge-density stripes in double-layer La${}_3$Ni${}_2$O${}_7$
• Spin-glass state in nickelate superconductors
• Orbital-selective spin-triplet superconductivity in infinite-layer LaNiO${}_2$
• Single-particle spectra and magnetic susceptibility in the Emery model: a dynamical mean-field perspective
• Floating zone growth at high oxygen pressures in Ruddlesden-Popper bilayer nickelate Y${}_y$Sr${}_{3-y}$Ni${}_{2-x}$Al${}_x$O${}_{7-\delta }$
• Coherent cellular dynamical mean-field theory: a real-space quantum embedding approach to disorder in strongly correlated electron systems
• Valency, charge-transfer, and orbital-dependent correlation in bilayer nickelates Nd3Ni2O7