Inorganic Chemistry, Vol.43, No.19, 6075-6082, 2004
Ferromagnetic anomaly associated with the antiferromagnetic transitions in (donor)[Ni(mnt)(2)]-type charge-transfer salts
Three newly prepared [Ni(mnt)(2)] complexes, (HMTTF)[Ni(mnt)(2)], (ChSTF)[Ni(mnt)(2)], and (DBTTF)(2)[Ni(mnt)(2)], are reported (DBTTF = dibenzotetrathiafulvalene, ChSTF = 2,3-cyclohexylenedithio-1,4-dithia-5,8-diselanafulvalene, HMTTF = bis(trimethylene)-tetrathiafulvalene, and mnt = maleonitrile dithiolate). The former two compounds have usual DA-type (D = donor, A = acceptor) mixed stacks, whereas the DBTTF complex has DDDDAA-type 6-fold columns. These compounds are electrical insulators, but the HMTTF and ChSTF complexes exhibit chiT minima at 16 and 55 K, respectively, followed by chiT peaks at 8 and 16 K. Below these temperatures the ESR signal disappears, indicating antiferromagnetic transitions. The origin of the ferromagnetic interaction is explained either from the difference of the g values between the donor and the anion or from the intrinsic ferromagnetic interaction of the [Ni(mnt)(2)] anions.