Entangled Electrons Drive a non-Superexchange Mechanism in a Cobalt Quinoid Dimer Complex

Abstract

A central theme in chemistry is the understanding of the mechanisms that drive chemical transformations. A well-known, highly cited mechanism in organometallic chemistry is the superexchange mechanism in which unpaired electrons on two or more metal centers interact through an electron pair of the bridging ligand. We use a combination of novel synthesis and computation to show that such interactions may in fact occur by a more direct mechanism than superexchange that is based on direct quantum entanglement of the two metal centers. Specifically, we synthesize and experimentally characterize a novel cobalt dimer complex with benzoquinoid bridging ligands and investigate its electronic structure with the variational two-electron reduced density matrix method using large active spaces. The result draws novel connections between inorganic mechanisms and quantum entanglement, thereby opening new possibilities for the design of strongly correlated organometallic compounds whose magnetic and spin properties have applications in superconductors, energy storage, thermoelectrics, and spintronics.

References in corpus (7)

• Quantum entanglement
• Quantum Computing in Molecular Magnets
• Perspective on density functional theory
• Structure of Fermionic Density Matrices: Complete N-representability Conditions
• Spin quantum tunneling via entangled states in a dimer of exchange coupled single-molecule magnets
• Single-Chain Magnets
• Strong Electron Correlation in Nitrogenase Cofactor, FeMoco

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