CASSCF and CASPT2 calculations of hole-doped amines with triplet carbene groups. Possibilities of high-Tc organic ferrimagnets

Ab initio CASSCF and CASPT2 calculations were carried out for hole-doped amines with triplet carbene groups such as monocations of bis(methylene) and tris(methylene) amines in order to confirm previous spin polarization (SP) and delocalization (SD) rules for ion-radicals. The ground states for the hole-doped bis(methylene) and tris(methylene) amines were calculated to be quartet and sextet, respectively. The low (LS)- and high (HS)-spin crossover occurred upon hole doping, being consistent with the SD rules. Implications of the calculated results are discussed in relation to possibilities of organic ferri- and ferro-magnets composed of CT complexes with radical substituents.