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[M(SCN)2(bopy)2], where M = Mn(II), Ni(II), Cu(II), and [CuCl2(bopy)2] complexes have been prepared and studied using IR, UV–Vis and EPR spectroscopy, and X-ray crystallography. 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.