Detailed electronic structure calculations of picene clusters doped by potassium modeling the crystalline K3picene structure show that while two electrons are completely transferred from potassium atoms to the LUMO of pristine picene, the third one r
emains closely attached to both material components. Multiconfigurational analysis is necessary to show that many structures of almost degenerate total energies compete to define the cluster ground state. Our results prove that the 4s orbital of potassium should be included in any interaction model describing the material. We propose a quarter filled two orbital model as the most simple model capable of describing the electronic structure of K-intercalated picene. Precise solutions obtained by a development of Lanczos method show low energy electronic excitations involving orbitals located at different positions. Consequently, metallic transport is possible in spite of the clear dominance of interaction over hopping.
Present routes to produce magnetic organic-based materials adopt a common strategy: the use of magnetic species (atoms, polyradicals, etc.) as building blocks. We explore an alternative approach which consists of selective hydrogenation of Polycyclic
Aromatic Hydrocarbons. Self-Consistent-Field (SCF) (Hartree-Fock and DFT) and multi-configurational (CISD and MCSCF) calculations on coronene and corannulene, both hexa-hydrogenated, show that the formation of stable high spin species is possible. The spin of the ground states is discussed in terms of the Hund rule and Liebs theorem for bipartite lattices (alternant hydrocarbons in this case). This proposal opens a new door to magnetism in the organic world.
