High-Temperature Compensated Ferrimagnetism in the Molecular Framework Cr(pyrazine)3

Molecule-based analogues of perovskites hold promise for emergent electronic and magnetic phenomena, yet examples with sufficiently strong correlations remain elusive. We report the synthesis of Cr(pyrazine)3, a cubic ReO3-type framework in which CrIII ions are bridged exclusively by pyrazine radical anions. The material hosts oxide-strength antiferromagnetic interactions, rivaling that of inorganic analogues and far surpassing known molecule-based perovskite analogues. Near-complete compensation of the CrIII and radical magnetic sublattices yields a weak but persistent magnetization extending above room temperature, establishing Cr(pyrazine)3 as a rare example of a low-defect, compensated ferrimagnet. The stability and simplicity of this molecule-based network make it an attractive platform for redox tuning, postsynthetic modification, and chemical vapor deposition, providing new opportunities to engineer strongly correlated behavior in molecular analogues of ReO3 and perovskite frameworks.