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Abstract
The valence intermediate effective Hamiltonian (VIEH) approach has become a powerful tool for dissecting the fundamental components of spin-state energetics in magnetically coupled system. Combined with differently sized complete active space approaches (CASSCF), this method enables a decomposition of the magnetic coupling constant J into its underlying physical contributions. Herein, we extend the VIEH framework to complexes with multiple magnetic coupling pathways. This approach is showcased with a homologous series of [M2(μ−O)(NH3)n]2+ complexes including Cu(II), Ni(II), and Fe(II). Typically, antiferromagnetic coupling progressively weakens from copper to nickel and iron. We demonstrate that this weakening arises primarily from an increase in the ferromagnetic coupling contribution across this series.
Supplementary materials
Title
Supporting Information
Description
1 Anisotropic Biquadratic Coupling Contributions
2 Computational Scaling of DDCI
3 Functional Dependence of Molecular Properties
4 Threshold Optimization in DDCI Calculations
5 Angular and Dihedral Dependence of σ, π & δ Orbitals
6 Fitting of U(δ) Parameters from Dihedral Scans
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