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The mutual coupling of spin and lattice degrees of freedom is ubiquitous inmagnetic materials and potentially creates exotic magnetic states in responseto the external magnetic field. Particularly, geometrically frustrated magnetsserve as a fertile playground for realizing magnetic superstructure phases.Here, we observe an unconventional two-step magnetostructural transition priorto a half-magnetization plateau in a breathing pyrochlore chromium spinel bymeans of state-of-the-art magnetization and magnetostriction measurements inultrahigh magnetic fields available up to 600 T. Considering a microscopicmagnetoelastic theory, the intermediate-field phase can be assigned to amagnetic superstructure with a three-dimensional periodic array of 3-up-1-downand canted 2-up-2-down spin molecules. We attribute the emergence of themagnetic superstructure to a unique combination of the strong spin-latticecoupling and large breathing anisotropy.

Signatures of a magnetic superstructure phase induced by ultrahigh magnetic fields in a breathing pyrochlore antiferromagnet