Correlated electron behavior of metalorganic molecules: insights from density functional theory combined with many-body effects using exact diagonalization

Abstract

A proper theoretical description of electronic structure of the 3d orbitals in the metal centers of functional metalorganics is a challenging problem. In this letter, we apply density functional theory and an exact diagonalization method in a many body approach to study the ground state electronic configuration of an iron porphyrin (FeP) molecule. Our study reveals that dynamical correlation effects are important, and FeP is a potential candidate for realizing a spin crossover due to a subtle balance of crystal field effects, on-site Coulomb repulsion and hybridization between the Fe d-orbitals and ligand N p-states. The mechanism of switching between two close lying electronic configurations of Fe-d orbitals is shown. We discuss the generality of the suggested approach and the possibility to properly describe the electronic structure and related low energy physics of the whole class of correlated metal centered organometallic molecules.

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Cited by in corpus (8)

• Tuning the coupling of an individual magnetic impurity to a superconductor: quantum phase transition and transport
• Comparative study of electronic and magnetic properties of $M$Pc ($M$ = Fe, Co) molecules physisorbed on 2D MoS${}_2$ and graphene
• Realistic theory of electronic correlations in nanoscopic systems
• Designing a mechanically driven spin-crossover molecular switch via organic embedding
• Visualizing Intramolecular Distortions as the Origin of Transverse Magnetic Anisotropy
• Role of charge transfer in hybridization-induced spin transition in metal-organic molecules
• Dynamical Screening of Local Spin Moments at Metal-Molecule Interfaces
• Self-energy self-consistent density functional theory plus dynamical mean field theory