Stein, Christopher J. and Pantazis, Dimitrios A. and Krewald, Vera (2019):
Orbital Entanglement Analysis of Exchange-Coupled Systems.
In: The Journal of Physical Chemistry Letters, ACS Publications, pp. 6762-6770, 10, ISSN 1948-7185,
DOI: 10.1021/acs.jpclett.9b02417,
[Online-Edition: https://pubs.acs.org/doi/10.1021/acs.jpclett.9b02417],
[Article]

Abstract

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.

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