Inorganic Chemistry

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



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.


Thumbnail image of paper.pdf

Supplementary material

Thumbnail image of supplemental.pdf
Thumbnail image of ReO_data.xlsx
ReO data
Thumbnail image of N2_data.xlsx
N2 data
Thumbnail image of FeOH_data.xlsx
FeOH data
Thumbnail image of V_data.xlsx
V data
Thumbnail image of V.txt
Thumbnail image of Re_O.txt
Re O
Thumbnail image of Fe_OH.txt