Symmetry and broken symmetries in molecular orbital descriptions of unstable molecules II. Alignment, flustration and tunneling of spins in mesoscopic molecular magnets

Abstract.

As an extention of previous work [Yamaguchi K (1983) J Mol Structure (Theochem) 103:101], our theoretical efforts toward molecular materials are briefly reviewed. Axial, helical and general (cone, tetrahedron, etc) spin structures of carbon clusters, manganese oxide clusters and iron-sulfur clusters were investigated using the classical Heisenberg model and generalized Hartree-Fock theory. The spin flustrations in the clusters were also studied in relation to theoretical descriptions of the magnetism and the chemical bonds in active sites of several enzymes. The macroscopic quantum tunneling and coherence of spins in the manganese oxide clusters were analyzed using the instanton model, and the tunneling rate of spins was calculated by the coherent state path integral method. The spin transitions induced by an external magnetic field were studied by the path integral Monte Carlo method. The theoretical results were explained in terms of the symmetry and broken symmetry of the wavefunctions in the mesoscopic molecular systems, which are intermediate in the scale factor. The results were also applied to molecular design of mesoscopic clusters of clusters in the intermediate and strong correlation regime. The active control of spins is finally discussed from the viewpoint of functionalities in molecular and biological materials, and technological applications of mesoscopic molecular magnets are discussed with regard to quantum computing.