Breathing pyrochlore magnet CuGaCr${}_4$S${}_8$: Magnetic, thermodynamic, and dielectric properties

Abstract

We investigate the crystallographic and magnetic properties of a chromium-based thiospinel CuGaCr${}_4$S${}_8$. From a synchrotron x-ray diffraction experiment and structural refinement, Cu and Ga atoms are found to occupy the tetrahedral $A$-sites in an alternate way, yielding breathing pyrochlore Cr network. CuGaCr${}_4$S${}_8$ undergoes a magnetic transition associated with a structural distortion at 31 K in zero magnetic field, indicating that the spin-lattice coupling is responsible for relieving the geometrical frustration. When applying a pulsed high magnetic field, a sharp metamagnetic transition takes place at 40 T, followed by a 1/2-magnetization plateau up to 103 T. These phase transitions accompany dielectric anomalies, suggesting the presence of helical spin correlations in low-field phases. The density-functional-theory calculation reveals that CuGaCr${}_4$S${}_8$ is dominated by antiferromagnetic and ferromagnetic exchange couplings within small and large tetrahedra, respectively, in analogy with CuInCr${}_4$S${}_8$. We argue that $A$-site-ordered Cr thiospinels serve as an excellent platform to explore diverse magnetic phases along with pronounced magnetoelastic and magnetodielectric responses.

arXiv comment12 pages, 13 figures

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