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.

arXiv comment11 pages, 8 figures, accepted in Journal of the Physical Society of Japan

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