Inorganic Chemistry

A Combined Spin-Flip and IP/EA Approach for Handling Spin and Spatial Degeneracies: Application to Double Exchange Systems

Nicholas Mayhall Virginia Tech

Abstract

Many multiconfigurational systems, such as single-molecule magnets, are difficult to study using traditional computational methods due to the simultaneous existence of both spin and spatial degeneracies. In this work, a new approach termed n-spin-flip Ionization Potential/Electron Affinity (nSF-IP or nSF-EA) is introduced which combines the spin-flip method of Anna Krylov with particle-number changing IP/EA methods. We demonstrate the efficacy of the approach by applying it to the strongly-correlated N2+ as well as several double exchange systems. We also demonstrate that when these systems are well-described by a double exchange model Hamiltonian, only 1SF-IP/EA is required to extract the double exchange parameters and accurately predict energies for the low-spin states. This significantly reduces the computational effort for studying such systems. The effects of including additional excitations (using a RAS-nSF-IP/EA scheme) are also examined, with particular emphasis on hole and particle excitations.

Content

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Supplementary material

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supplemental
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ReO data
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N2 data
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FeOH data
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V data
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V
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Re O
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Fe OH