Cluster-Spin-Glass Magnetic Behavior and Morphology in the Coordination Polymer Alloys Fe_yCo_1-yBTT

We report the synthesis of a series of pseudo-1D coordination polymer (CP) materials with the formula Fe_yCo_1-yBTT (BTT = 1,3,5-benzenetrithiolate). These materials were structurally characterized by PXRD Rietveld, EXAFS, and PDF analyses, revealing that the CP superstructure enables a continuous and isomorphous alloy between the two homometallic compounds. Lower Fe loadings exhibit emergent spin glass magnetic behavior, such as memory effects and composition-dependent spin glass response time constants ranging from 6.9 × 10^-9 s to 1.8 × 10^-6 s. These data are consistent with the formation of spin clusters within the lattice. The magnetic behavior in these materials was modeled via replica exchange Monte Carlo simulation, which provides a good match for the experimentally measured spin glassing and magnetic phase transitions. These findings underscore how the rigid superstructure of CP and MOF scaffolds can enable the systematic tuning of physical properties, such as the spin glass behavior described here.