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

TL;DR

This study combines experimental measurements and advanced theoretical modeling to reveal that LaNiO₂ exhibits short-range magnetic correlations and non-Curie-Weiss susceptibility behavior, akin to doped cuprates, despite lacking long-range magnetic order.

Contribution

It provides a comprehensive multi-method analysis of magnetic correlations in LaNiO₂, linking experimental observations with theoretical insights from Hubbard model simulations.

Findings

Absence of long-range magnetic order down to 2 K.

Presence of short-range magnetic correlations and glassy spin dynamics.

Intrinsic susceptibility shows non-Curie-Weiss behavior at high temperatures.

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.