Magnetostructural Dynamics from Hubbard-U Corrected Spin-Projection: [2Fe-2S] Complex in Ferredoxin.

A Hubbard-corrected spin-projected two-determinant approach, EBS+Uscf, is introduced to treat low-spin ground states of antiferromagnetically coupled transition metal complexes. In addition to providing access to total energies, forces, and ab initio simulations, it allows one to readily compute Heisenberg's exchange coupling J(t) on the fly. By studying the binuclear [2Fe-2S] cofactor in a metalloprotein, Anabaena Fd, within this consistent nonempirical procedure in combination with a QM/MM framework, it is illustrated that spin-projection, self-interaction corrections, thermal fluctuations, and protein matrix shifts are crucial in obtaining ⟨J⟩ close to the experiment.