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.

18 pages, 14 figures

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• 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