Ground State of the Fe(II)-porphyrin Model System Corresponds to the Quintet State: A DFT and DMRG-based Tailored CC Study

Abstract

Fe(II)-porphyrins (FeP) play an important role in many reactions relevant to material science and biological processes, due to their closely lying spin states. However, this small energetic separation also makes it challenging to establish the correct spin state ordering. Although the prevalent opinion is that these systems posses the triplet ground state, the recent experiment on Fe(II)-phthalocyanine under conditions matching those of an isolated molecule points toward the quintet ground state. We present a thorough study of FeP model by means of the density functional theory and density matrix renormalization group based tailored coupled clusters, in which we address all previously discussed correlation effects. We examine the importance of geometrical parameters, the Fe-N distances in particular, and conclude that the system possesses the quintet ground state, which is in our calculations well-separated from the triplet state.

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• DMRG-tailored coupled cluster method in the 4c-relativistic domain: General implementation and application to the NUHFI and NUF${}_3$ molecules