We report thermal expansion and magnetostriction in breathing pyrochlore magnets LiACr4X8 (A = Ga, In, X = O, S) measured by a dilatometric method on sintered samples. All four of these compounds showed a large volume contraction associated with antiferromagnetic order with decreasing temperature. Above the Neél temperature, LiGaCr4S8 showed negative thermal expansion, LiInCr4O8 showed positive thermal expansion with concave-downward temperature dependence, and LiInCr4S8 showed positive forced volume magnetostriction. All these phenomena are likely caused by the complex structure-magnetism correlation within the breathing pyrochlore structure with J and J'. These results suggested that breathing pyrochlore magnets are promising for the realization of various volumetric phenomena related to their magnetism not only in the magnetically-ordered phase but also in the paramagnetic phase.

Strain induced by a magnetic field is a common phenomenon for ferromagnets, but few antiferromagnets show large strain induced by a magnetic field. On the basis of linear strain measurements of sintered samples of triangular antiferromagnet ACrS2 (A = Cu, Ag, and Au) in magnetic fields up to 9 T, the AgCrS2 sample was found to show a large strain, yielding a large volume change over 700 ppm, which is one of the largest volume changes measured to date for an antiferromagnet. This large strain appeared only at the Néel temperature of 42 K and was not restored to its initial state when the applied magnetic field was decreased to zero; however, it was initialized by cooling the sample to far below the Néel temperature. These results suggest that the coexistence of magnetically ordered and paramagnetic phases at the first-order phase transition plays an important role. AuCrS2 showed a magnetic-field-induced strain with similar features, although it was smaller than that in AgCrS2.

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Sintered samples of Cr3Te4 and Cr2Te3 are found to show large strains accompanied by large volume changes under a magnetic field. In Cr3Te4, volume increases of Δ V/ V =  500–1170 ppm by applying a magnetic field of 9 T are observed over the entire temperature range below 350 K. At room temperature, the Δ V/ V value exceeds 1000 ppm, which is considerably larger than the maximum values reported for Cr-based magnets, thus far, and is comparable to the room-temperature value of forced-volume magnetostriction in invar alloys. Cr2Te3 shows a large Δ V/ V of 680 ppm when applying a magnetic field of 9 T at 200 K. Both samples display particularly large volume increases around the Curie temperature, where they also show negative thermal expansion due to the microstructural effects, suggesting that the cooperation between anisotropic lattice deformation associated with the magnetic ordering and microstructural effects is essential for the manifestation of the large magnetic-field-induced volume changes.