A high-frequency EPR characterization of the S = 2 linear tri-atomic chain in Cr3(dpa)4Cl2·CH2Cl2

► Well resolved EPR signals on complex Cr3(dpa)4Cl2·CH2Cl2 are observed by HF-EPR. ► Axial zero-field splitting parameter D is found to be large negative of −1.643 cm−1. ► Cr3(dpa)4Cl2·CH2Cl2 has a well defined spin ground state at room temperature.