Modulated spin helicity stabilized by incommensurate orbital density waves in a quadruple perovskite manganite

TL;DR

This study combines neutron diffraction and Landau theory to elucidate the complex spin and orbital ordering in CaMn7O12, revealing a modulated spin helicity stabilized by incommensurate orbital density waves in a multiferroic material.

Contribution

It introduces a phenomenological model explaining the spin and orbital coupling and the magnetic structure in CaMn7O12, highlighting the role of incommensurate orbital density waves.

Findings

The ground state features a nearly-constant-moment helix with modulated helicity.

Orbital density waves influence the spin structure via magneto-orbital coupling.

The model explains the temperature-dependent polarization and absence of dielectric anomalies.

Abstract

Through a combination of neutron diffraction and Landau theory we describe the spin ordering in the ground state of the quadruple perovskite manganite CaMn7O12 - a magnetic multiferroic supporting an incommensurate orbital density wave that onsets above the magnetic ordering temperature, TN1 = 90 K. The multi-k magnetic structure in the ground state was found to be a nearly-constant-moment helix with modulated spin helicity, which oscillates in phase with the orbital occupancies on the Mn3+ sites via trilinear magneto-orbital coupling. Our phenomenological model also shows that, above TN2 = 48 K, the primary magnetic order parameter is locked into the orbital wave by an admixture of helical and collinear spin density wave structures. Furthermore, our model naturally explains the lack of a sharp dielectric anomaly at TN1 and the unusual temperature dependence of the electrical polarisation.