Multiconfiguration Pair-Density Functional Theory Predicts Spin-State Ordering in Iron Complexes with the Same Accuracy as Complete Active Space Second-Order Perturbation Theory at a Significantly Reduced Computational Cost

Liam Wilbraham, Pragya Verma, Donald G. Truhlar, Laura Gagliardi, Ilaria Ciofini

Research output: Contribution to journalArticlepeer-review

30 Scopus citations

Abstract

The spin-state orderings in nine Fe(II) and Fe(III) complexes with ligands of diverse ligand-field strength were investigated with multiconfiguration pair-density functional theory (MC-PDFT). The performance of this method was compared to that of complete active space second-order perturbation theory (CASPT2) and Kohn-Sham density functional theory. We also investigated the dependence of CASPT2 and MC-PDFT results on the size of the active-space. MC-PDFT reproduces the CASPT2 spin-state ordering, the dependence on the ligand field strength, and the dependence on active space at a computational cost that is significantly reduced as compared to CASPT2.

Original languageEnglish (US)
Pages (from-to)2026-2030
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume8
Issue number9
DOIs
StatePublished - May 4 2017

Bibliographical note

Funding Information:
This work was supported in part (L.G. and D.G.T.) by the AFOSR Grant FA9550-16-1-0134. I.C. received funding from the European Research Council (ERC) under the European Union?s Horizon 2020 research and innovation program (Grant Agreement No. 648558, STRIGES CoG grant).

Publisher Copyright:
© 2017 American Chemical Society.

Copyright:
Copyright 2017 Elsevier B.V., All rights reserved.

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