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, 10, pp. 6762-6770. ACS Publications, ISSN 1948-7185,
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.
| Item Type: | Article |
|---|---|
| Erschienen: | 2019 |
| Creators: | Stein, Christopher J. and Pantazis, Dimitrios A. and Krewald, Vera |
| Title: | Orbital Entanglement Analysis of Exchange-Coupled Systems |
| Language: | English |
| 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. |
| Journal or Publication Title: | The Journal of Physical Chemistry Letters |
| Journal volume: | 10 |
| Publisher: | ACS Publications |
| Divisions: | 07 Department of Chemistry Zentrale Einrichtungen Zentrale Einrichtungen > University IT-Service and Computing Centre (HRZ) Zentrale Einrichtungen > University IT-Service and Computing Centre (HRZ) > Hochleistungsrechner 07 Department of Chemistry > Theoretische Chemie |
| Date Deposited: | 30 Oct 2019 07:39 |
| DOI: | 10.1021/acs.jpclett.9b02417 |
| Official URL: | https://pubs.acs.org/doi/10.1021/acs.jpclett.9b02417 |
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