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Spin State Ordering in Metal-Based Compounds Using the Localized Active Space Self-Consistent Field Method

preprint
submitted on 19.07.2019 and posted on 22.07.2019 by Riddhish Pandharkar, Matthew R. Hermes, Christopher J. Cramer, Laura Gagliardi

Quantitatively accurate calculations for spin state ordering in transition-metal complexes typically demand a robust multiconfigurational treatment. The poor scaling of such methods with increasing size makes them impractical for large, strongly correlated systems. Density matrix embedding theory (DMET) is a fragmentation approach that can be used to specifically address this challenge. The single-determinantal bath framework of DMET is applicable in many situations, but it has been shown to perform poorly for molecules characterized by strong correlation when a multiconfigurational self-consistent field solver is used. To ameliorate this problem, the localized active space self-consistent field (LASSCF) method was recently described. In this work, LASSCF is applied to predict spin state energetics in mono- and di-iron systems and we show that the model offers an accuracy equivalent to CASSCF but at a substantially lower computational cost. Performance as a function of basis set and active space is also examined.

History

Email Address of Submitting Author

pandh009@umn.edu

Institution

University of Minnesota

Country

USA

ORCID For Submitting Author

0000-0003-4086-4308

Declaration of Conflict of Interest

No conflict of interest

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