Orbital Configurations and Magnetic Properties of Double-Layered Antiferromagnet Cs3Cu2Cl4Br3

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  • Orbital Configurations and Magnetic Properties of Double-Layered Antiferromagnet Cs<SUB>3</SUB>Cu<SUB>2</SUB>Cl<SUB>4</SUB>Br<SUB>3</SUB>

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We report the single-crystal X-ray analysis and magnetic properties of a new double-layered perovskite antiferromagnet, Cs3Cu2Cl4Br3. This structure is composed of Cu2Cl4Br3 double layers with elongated CuCl4Br2 octahedra and is closely related to the Sr3Ti2O7 structure. An as-grown crystal has a singlet ground state with a large excitation gap of Δ⁄kB\\simeq2000 K, due to the strong antiferromagnetic interaction between the two layers. Cs3Cu2Cl4Br3 undergoes a structural phase transition at Ts\\simeq330 K accompanied by changes in the orbital configurations of Cu2+ ions. Once a Cs3Cu2Cl4Br3 crystal is heated above Ts, its magnetic susceptibility obeys the Curie–Weiss law with decreasing temperature even below Ts and does not exhibit anomalies at Ts. This implies that in the heated crystal, the orbital state of the high-temperature phase remains unchanged below Ts, and thus, this orbital state is the metastable state. The structural phase transition at Ts is characterized as an order–disorder transition of Cu2+ orbitals.

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