Complex magnetic phase diagram with a small phase pocket in a three-dimensional frustrated magnet CuInCr$_{4}$S$_{8}$

Abstract

Frustrated magnets with a strong spin-lattice coupling can show rich magnetic phases and the associated fascinating phenomena. A promising platform is the breathing pyrochlore magnet CuInCr$_{4}$S$_{8}$ with localized $S=3/2$ Cr$^{3+}$ ions, which is proposed to be effectively viewed as an $S=6$ Heisenberg antiferromagnet on the face-centered-cubic lattice. Here, we unveil that CuInCr$_{4}$S$_{8}$ exhibits a complex magnetic phase diagram with a small phase pocket ($A$ phase) by means of magnetization, magnetostriction, magnetocapacitance, and magnetocaloric-effect measurements in pulsed high magnetic fields of up to 60 T. Remarkably, the appearance of $A$ phase is accompanied by anomalous magnetostrictive and magnetocapacitive responses, suggesting the emergence of helimagnetism in contrast to the neighboring commensurate magnetic phases. Besides, the high-entropy nature is confirmed in the high-temperature side of $A$ phase. These features are potentially related to a thermal fluctuation-driven multiple-$q$ state caused by the magnetic frustration, which has been theoretically predicted but yet experimentally undiscovered.