Magnetic order and dynamics of the charge-ordered antiferromagnet La1.5Sr0.5CoO4

TL;DR

This study uses neutron scattering to analyze the magnetic order and excitations in La1.5Sr0.5CoO4, revealing a complex interplay of charge order, magnetic correlations, and spin dynamics consistent with a spin-wave model.

Contribution

It provides a detailed experimental and theoretical characterization of magnetic excitations in a charge-ordered cobaltate, including the validation of a spin-wave theory for high-spin Co2+ ions.

Findings

Magnetic order appears below 31 K with a kink in susceptibility.

Magnetic excitation spectrum matches spin-wave theory predictions.

Co3+ ions are non-magnetic, supporting S=0 state.

Abstract

We describe neutron scattering experiments performed to investigate the magnetic order and dynamics of half-doped La1.5Sr0.5CoO4. This layered perovskite exhibits a near-ideal checkerboard pattern of Co2+/Co3+ charge order at temperatures below ~ 800 K. Magnetic correlations are observed at temperatures below ~ 60 K but static magnetic order only becomes established at 31 K, a temperature at which a kink is observed in the susceptibility. On warming above 31 K we observed a change in the magnetic correlations which we attribute either to a spin canting or to a change in the proportion of inequivalent magnetic domains. The magnetic excitation spectrum is dominated by an intense band extending above a gap of approximately 3 meV up to a maximum energy of 16 meV. A weaker band exists in the energy range 20-30 meV. We show that the excitation spectrum is in excellent quantitative agreement with the predictions of a spin-wave theory generalized to include the full magnetic degrees of freedom of high-spin Co2+ ions in an axially distorted crystal field, coupled by Heisenberg exchange interactions. The magnetic order is found to be stabilized by dominant antiferromagnetic Co2+ -- Co2+ interactions acting in a straight line through Co3+. No evidence is found for magnetic scattering from the Co3+ ions, supporting the view that Co3+ is in the S = 0 state in this material.