The dissociation catastrophe in fluctuating-charge models and its implications for the concept of atomic electronegativity

Physics – Chemical Physics

Scientific paper

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17 pages, prepared for "Proceedings of QSCP-XIII" in Prog. Theor. Chem. Phys

Scientific paper

10.1007/978-90-481-2596-8_19

We have recently developed the QTPIE (charge transfer with polarization current equilibration) fluctuating-charge model, a new model with correct dissociation behavior for nonequilibrium geometries. The correct asymptotics originally came at the price of representing the solution in terms of charge-transfer variables instead of atomic charges. However, we have found an exact reformulation of fluctuating-charge models in terms of atomic charges again, which is made possible by the symmetries of classical electrostatics. We show how this leads to the distinguishing between two types of atomic electronegativities in our model. While one is a intrinsic property of individual atoms, the other takes into account the local electrical surroundings. This suggests that this distinction could resolve some confusion surrounding the concept of electronegativity as to whether it is an intrinsic property of elements, or otherwise.

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