Abstract

AbstractTwo new TTF‐based ligands involving terpyridine moiety (L1=4‐(4′‐Methyl‐phenyl‐2,2 : 6’,2’’‐terpyridine −4‐ylmethylthio)‐5‐(2‐cyanoethylthio)‐4′,5′‐bis(methylthio)tetrathiafulvene and L2=4‐(4′‐Methyl‐phenyl‐2,2 : 6’,2’’‐terpyridine −4‐ylmethylthio)‐5‐(2‐cyanoethylthio)‐4′,5′‐bis(propylthio)tetrathiafulvene) have been synthesized and seven related mononuclear complexes were isolated as single crystals. The 2 : 1 (ligand : metal) complexes of formula [Co(L1)2](NO3)2 (2) and [Co(L1)2](BF4)2 (3) displayed thermal spin crossover transition while the 1 : 1 complexes of formula [CoCl2(L1)](DMF)2 (4), [CoBr2(L1)] ⋅ (DMF) (5), [CoCl2(L2)] ⋅ (DMF) ⋅ 0.5(Et2O) (6) and [CoBr2(L2)] ⋅ (DMF) (7) displayed slow magnetic relaxation through either Raman or Raman/Direct combination processes. A relationship between the structure and the nature of the magnetic relaxation processes is proposed.

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