Chemical bonds and spin state splittings in spin crossover complexes. A DFT and QTAIM analysis

Density functional theory (DFT) calculations have been performed for the high-spin (HS) and low-spin (LS) isomers of a series of iron(H) spin crossover complexes with nitrogen ligands. The calculated charge densities have been analyzed in the framework of the quantum theory of atoms in molecules QTAIM). For a number of iron(H) complexes with substituted tris(pyrazolyl) ligands the energy difference between HS and LS isomers, the spin state splitting, has been decomposed into atomic contributions in order to rationalize changes of the spin state splitting due to substituent effects.