Having demonstrated that angular scans and subsequent decoupling of the ferromagnetic and antiferromagnetic components are feasible for both the copper and nickel complexes, we now turn to the iron complex, which features the largest number of coupling paths in this study. While the overall pattern of the angle scans is similar to the copper and nickel complexes (see Figure , top), the larger number of magnetic coupling paths leads to a significant reduction in the overall J coupling variation across all scans. In the iron complex, the J coupling changes are ∆J CAS,Fe = 0.10 cm -1 and ∆J BS-DFT,Fe = 0.04 cm -1 , nearly vanishing within the numerical precision. This precludes a meaningful multiple linear regression approach since the small differences in the overall J coupling correspond to an equally small variation in orbital overlaps during the scan. Recently, Heyer and coworkers demonstrated that by rotating the ligand spheres in µ-oxo-bridged copper complexes relative to each other, it is possible to switch the J coupling from strongly antiferromagnetic for collinear magnetic orbitals to strongly ferromagnetic for nearly orthogonal magnetic orbitals. Following this approach, we performed an M -O -M -N dihedral scan in 5 • steps across a ±30 • range around the minimum at 31.0 • . This significantly increased the variation in the J coupling, reaching ∆J CAS,Fe = 1.01 cm -1 and ∆J BS-DFT,Fe = 1.43 cm -1 (see Figure , bottom), pushing the results beyond the numerical error range of both CASSCF and BS-DFT calculations.