The Many-Electron Perspective on Local Spins and their Implication for Chemical Bonding

is analyzed directly. Within this framework, the influence of spin multiplicity is explicitly accounted for. The method is applied to a range of molecules containing first-row elements and hydrogen. The analysis reveals that covalent bonding is directly reflected in the exchange of opposite-spin electrons, manifesting as redistributions of the local spin weights. Furthermore, local spin distributions tending toward higher local spin states are associated with increased electron delocalization. Clear connections between local spin distributions, molecular geometry, the hybridization model, and molecular orbital theory are established. This real-space definition establishes a theory-independent, real-space framework in which local spins and chemical bonding can be understood directly from the many-electron wave function.

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Publication Details

Journal
Journal of Chemical Theory and Computation
Published
2026-07-26
DOI
https://doi.org/10.1021/acs.jctc.6c00997
Primary Topic
Magnetism in coordination complexes
Type
article
Field-Weighted Citation Impact
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article

The Many-Electron Perspective on Local Spins and their Implication for Chemical Bonding

Michel V. Heinz, Arne Lüchow, Nicole Maser
Journal of Chemical Theory and Computation
Magnetism in coordination complexes
article

The Many-Electron Perspective on Local Spins and their Implication for Chemical Bonding

Michel V. Heinz, Arne Lüchow, Nicole Maser
article en

Abstract

is analyzed directly. Within this framework, the influence of spin multiplicity is explicitly accounted for. The method is applied to a range of molecules containing first-row elements and hydrogen. The analysis reveals that covalent bonding is directly reflected in the exchange of opposite-spin electrons, manifesting as redistributions of the local spin weights. Furthermore, local spin distributions tending toward higher local spin states are associated with increased electron delocalization. Clear connections between local spin distributions, molecular geometry, the hybridization model, and molecular orbital theory are established. This real-space definition establishes a theory-independent, real-space framework in which local spins and chemical bonding can be understood directly from the many-electron wave function.

Journal of Chemical Theory and Computation
RWTH Aachen University (DE)
Openalex Percentile: Top 22%
Magnetism in coordination complexes
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The Many-Electron Perspective on Local Spins and their Implication for Chemical Bonding — Michel V. Heinz, Arne Lüchow, et al. · Journal of Chemical Theory and Computation (2026) | TGRS Research Map | TGRS