Ferromagnetism in Co7(TeO3)4Br6: A byproduct of complex antiferromagnetic order and single-ion anisotropy

TL;DR

This study reveals complex magnetic behavior in Co7(TeO3)4Br6, including incommensurate antiferromagnetic order, a transition to ferrimagnetism, and unusual anisotropic hysteresis, driven by competing interactions and single-ion anisotropy.

Contribution

It provides detailed neutron diffraction and magnetic measurements showing how complex magnetic phases emerge from competing interactions in a new oxi-halide compound.

Findings

Incommensurate antiferromagnetic order at 34 K

Transition to ferrimagnetic structure at 27 K

Unusual anisotropic magnetic hysteresis behavior

Abstract

Pronounced anisotropy of magnetic properties and complex magnetic order of a new oxi-halide compound Co7(TeO3)4Br6 has been investigated by powder and single crystal neutron diffraction, magnetization and ac susceptibility techniques. Anisotropy of susceptibility extends far into the paramagnetic temperature range. A principal source of anisotropy are anisotropic properties of the involved octahedrally coordinated single Co(2+) ions, as confirmed by angular-overlap-model calculations presented in this work. Incommensurate antiferromagnetic order sets in at TN=34 K. Propagation vector is strongly temperature dependent reaching k1=(0.9458(6), 0, 0.6026(5)) at 30 K. A transition to a ferrimagnetic structure with k2=0 takes place at TC=27 K. Magnetically ordered phase is characterized by very unusual anisotropy as well: while M-H scans along b-axis reveals spectacularly rectangular but otherwise standard ferromagnetic hysteresis loops, M-H studies along other two principal axes are perfectly reversible, revealing very sharp spin flop (or spin flip) transitions, like in a standard antiferromagnet (or metamagnet). Altogether, the observed magnetic phenomenology is interpreted as an evidence of competing magnetic interactions permeating the system, first of all of the single ion anisotropy energy and the exchange interactions. Different coordinations of the Co(2+)-ions involved in the low-symmetry C2/c structure of Co7(TeO3)4Br6 render the exchange-interaction network very complex by itself. Temperature dependent changes in the magnetic structure, together with an abrupt emergence of a ferromagnetic component, are ascribed to continual spin reorientations described by a multi-component, but yet unknown, spin Hamiltonian.