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

Riddhish Pandharkar, Matthew R. Hermes, Chris Cramer, Laura Gagliardi

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

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 that of CASSCF but at a substantially lower computational cost. Performance as a function of basis set and active space is also examined.

Original languageEnglish (US)
Pages (from-to)5507-5513
Number of pages7
JournalJournal of Physical Chemistry Letters
DOIs
StateAccepted/In press - Jan 1 2019

PubMed: MeSH publication types

  • Journal Article

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