New [M(SCN)(2)(L)(4)] complexes, where M = Mn(II), Ni(II),Cu(II)and L = 1-methylimidazole have been synthesized. The electronic structures of the complexes were calculated using the DFT method, and the descriptions of frontier molecular orbitals and the relocation of the electron density of the compounds were determined. The crystal field splitting, Racah repulsion and nephelauxetic parameters were determined from the electronic spectra of the complexes. The magnetic properties revealed almost ideal paramagnetism for all the complexes under study, evidenced by values close to zero for both the Curie-Weiss temperature and the imaginary part of the ac magnetic susceptibility. (c) 2012 Elsevier Ltd. All rights reserved.