Two crystal polymorphs of Ni(cyclam)I (cyclam = 1,4,8,11-tetraazacyclotetradecane) were synthesized, and their magnetic properties were investigated. Temperature-dependent X-ray structural analysis and magnetic measurements revealed gradual spin transition in molecular-crystal polymorph -[Ni(cyclam)I] (), whereas the zigzag-chain polymorph -[Ni(cyclam)(μ-I)]I () did not show an obvious spin transition. The entropy difference between high- and low-spin states of estimated by assuming the spin-equilibrium model is much smaller than those in typical iron(II)-based spin-crossover (SCO) complexes, suggesting that the normal mode softening is less remarkable in . In this system, it is clearly evidenced that the interaction mode responsible to the spin equilibrium in octahedral nickel(II) complexes is highly anistropic, i.e., -elongation and ,-shortening of the coordination octahedron.
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