Frustrated $J_1-J_2$ Diamond Lattice Antiferromagnet Co${}_2$Ti${}_3$O${}_8$ with a Vacancy-ordered Spinel Structure Synthesized via a Topochemical Reaction

Abstract

Metastable Co${}_2$Ti${}_3$O${}_8$ was synthesized through a topochemical reaction using Li${}_2$CoTi${}_3$O${}_8$ as the precursor, resulting in a vacancy-ordered spinel structure. Crystal structure analysis confirmed that Co ions selectively occupy the A-site, giving rise to a frustrated diamond lattice. Magnetic susceptibility and heat capacity measurements revealed antiferromagnetic order at 4.4 K, which is markedly suppressed compared to the negative Weiss temperature of $\sim -27$ K, indicating a high degree of frustration effects. Pulsed high-field magnetization measurements revealed a four-step successive magnetic phase transition, demonstrating that Co${}_2$Ti${}_3$O${}_8$ is a promising candidate for a frustrated $J_1-J_2$ diamond lattice. Additionally, the $J_2/J_1$ ration estimated from the molecular field approximation suggests the possibility of a spiral ordered ground state. These observations highlight the potential of frustrated magnetism in ordered spinel structures to expand the material search space for quantum magnetism, including magnetic skyrmions.

11 pages, 8 figures, accepted in Journal of the Physical Society of Japan

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