Energy Sciences

A new tool for the interpretation of multiconfigurational wave functions representing the spin states of exchange-coupled transition metal complexes is introduced. Based on orbital entanglement measures, herein derived from multiconfigurational density matrix renormalization group calculations, the complexity of the wave function is reduced, thus facilitating a connection with established concepts for the interpretation of magnetically coupled systems. We show that the entanglement of localized orbitals with a small basis set is a good representation of the magnetic coupling topology and that it is sensitive to chemical changes in homologous complexes. Furthermore, we introduce a measure for the magnetic relevance of orbitals in the active subspace and a concept for the quantitative comparison of different chemical species. The approach presented here will be easily applicable to higher nuclearity clusters, providing a direct insight into all states of the Heisenberg spin ladder for systems previously accessible only by single-configurational methods.