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On the connection between probability density analysis, QTAIM, and VB theory

Leonard Reuter, Arne Lüchow

2020Physical Chemistry Chemical Physics28 citationsDOI

Abstract

Classification of bonds is essential for understanding and predicting the reactivity of chemical compounds. This classification mainly manifests in the bond order and the contribution of different Lewis resonance structures. Here, we outline a first principles approach to obtain these orders and contributions for arbitrary wave functions in a manner that is both, related to the quantum theory of atoms in molecules and consistent with valence bond theory insight: the Lewis structures arise naturally as attractors of the all-electron probability density |Ψ|2. Doing so, we introduce a valence bond weight definition that does not collapse in the basis set limit.

Topics & Concepts

Valence bond theoryDensity functional theoryAtoms in moleculesConnection (principal bundle)Electron densityValence (chemistry)MoleculeStatistical physicsValence electronChemistryTheoretical physicsComputational chemistryQuantum mechanicsMathematicsPhysicsElectronGeometryMolecular orbitalAdvanced Chemical Physics StudiesMolecular spectroscopy and chiralitySpectroscopy and Quantum Chemical Studies