Short-range magnetic interactions and spin-glass behavior in the quasi-2D nickelate Pr4Ni3O8

TL;DR

This study investigates the magnetic properties of Pr4Ni3O8, revealing complex spin-glass behavior and multiple magnetic interactions that may hinder superconductivity in this quasi-2D nickelate.

Contribution

The paper reports the synthesis and detailed magnetic characterization of Pr4Ni3O8, highlighting its spin-glass behavior and multiple magnetic processes, which are novel findings for this material.

Findings

Pr4Ni3O8 exhibits spin-glass behavior with a freezing temperature around 68 K.

Muon-spin rotation indicates two distinct magnetic relaxation processes.

Complex magnetic interactions may negatively impact potential superconductivity.

Abstract

The nickelate Pr4Ni3O8 features quasi-two-dimensional layers consisting of three stacked square-planar NiO2 planes, in a similar way to the well-known cuprate superconductors. The mixed-valent nature of Ni and its metallic properties makes it a candidate for potentially unconventional superconductivity. We have synthesized Pr4Ni3O8 by topotactic reduction of Pr4Ni3O10 in 10 percent hydrogen gas, and report on measurements of powder-neutron diffraction, magnetization and muon-spin rotation (uSR). We find that Pr4Ni3O8 shows complicated spin-glass behavior with a distinct magnetic memory effect in the temperature range from 2 to 300 K and a freezing temperature T_s ~ 68 K. Moreover, the analysis of uSR spectra indicates two magnetic processes characterized by remarkably different relaxation rates: a slowly-relaxing signal, resulting from paramagnetic fluctuations of Pr/Ni ions, and a fast-relaxing signal, whose relaxation rate increases substantially below ~ 70 K which can be ascribed to the presence of short-range correlated regions. We conclude that the complex spin-freezing process in Pr4Ni3O8 is governed by these multiple magnetic interactions. It is possible that the complex magnetism in Pr4Ni3O8 is detrimental to the occurrence of superconductivity.