Jahn-Teller Inactivity and Magnetic Frustration in GeCo$_2$O$_4$ Probed by Ultrasound Velocity Measurements

TL;DR

This study uses ultrasound velocity measurements to explore the magnetic and orbital properties of GeCo$_2$O$_4$, revealing Jahn-Teller inactivity and bond frustration linked to orbital degeneracy and magnetic structure.

Contribution

It demonstrates the absence of Jahn-Teller activity despite orbital degeneracy and identifies the exchange path anisotropy and orbital frustration mechanisms in GeCo$_2$O$_4$.

Findings

Jahn-Teller inactivity despite orbital degeneracy.

Exchange path anisotropy along [111] direction.

Orbital frustration due to geometrical orbital interactions.

Abstract

Ultrasound velocity measurements of cubic spinel GeCo$_2$O$_4$ in single crystal were performed for the investigation of shear and compression moduli. The shear moduli in the paramagnetic state reveal an absence of Jahn-Teller activity despite the presence of orbital degeneracy in the Co$^{2+}$ ions. Such a Jahn-Teller inactivity indicates that the intersite orbital-orbital interaction is much stronger than the Jahn-Teller coupling. The compression moduli in the paramagnetic state near the N$\acute{e}$el temperature $T_N$ reveal that the most relevant exchange path for the antiferromagnetic transition lies in the [111] direction. This exchange-path anisotropy is consistent with the antiferromagnetic structure with the wave vector $q \parallel$ [111], suggesting the presence of bond frustration due to competition among a direct ferromagnetic and several distant-neighbors antiferromagnetic interactions. In the JT-inactive condition, the bond frustration can be induced by geometrical orbital frustration of $t_{2g}$-$t_{2g}$ interaction between the Co$^{2+}$ ions which can be realized in the pyrochlore lattice of the high spin Co$^{2+}$ with $t_{2g}$-orbital degeneracy. In GeCo$_2$O$_4$, the tetragonal elongation below $T_N$ releases the orbital frustration by quenching the orbital degeneracy.