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We report spin-singlet formation in an organic-inorganic hybrid identified as CH 3NH3Cu2Cl5. The hybrid adopts a layered structure in which Cu2Cl5− layers are separated by CH 3 NH3+ layers. The inorganic layers consist of corner- and edge-sharing CuCl6 octahedra, forming edge-sharing tetramers. Magnetic susceptibility measurements indicate strong antiferromagnetic interactions within the tetramers, whereas the coupling between the tetramers is weak. Low-temperature magnetic susceptibility data as well as electron spin resonance measurements suggest a nonmagnetic ground state with a large spin gap of ∼130K, in apparent contradiction with ferromagnetic interactions between nearest-neighbor spins. We discuss a spin-tetramer model in which antiferromagnetic next-nearest-neighbor interactions lead to a spin-singlet state.

physical review materials

Spin-singlet formation in the spin-tetramer layered organic-inorganic hybrid<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi>CH</mml:mi><mml:mn>3</mml:mn></mml:msub><mml:msub><mml:mi>NH</mml:mi><mml:mn>3</mml:mn></mml:msub><mml:msub><mml:mi>Cu</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi>Cl</mml:mi><mml:mn>5</mml:mn></mml:msub></mml:mrow></mml:math>

Spin-singlet formation in the spin-tetramer layered organic-inorganic hybridCH3NH3Cu2Cl5