Shannon entropy variation as a global indicator of electron density contraction at interatomic regions in chemical reactions.

Autor: Barrales-Martínez C; Instituto de Investigación Interdisciplinaria (I3), Vicerrectoría Académica, Universidad de Talca, Campus Talca, Talca, Chile. cesar.barrales@utalca.cl.; Centro de Bioinformática, Simulación y Modelado (CBSM), Facultad de Ingeniería, Universidad de Talca, Campus Talca, Talca, Chile. cesar.barrales@utalca.cl., Durán R; Facultad de Ciencias, Departamento de Química Ambiental, Universidad Católica de la Santísima Concepción, Concepción, Chile. rbduran@ucsc.cl., Caballero J; Centro de Bioinformática, Simulación y Modelado (CBSM), Facultad de Ingeniería, Universidad de Talca, Campus Talca, Talca, Chile.
Jazyk: angličtina
Zdroj: Journal of molecular modeling [J Mol Model] 2024 Oct 09; Vol. 30 (11), pp. 371. Date of Electronic Publication: 2024 Oct 09.
DOI: 10.1007/s00894-024-06171-0
Abstrakt: Context: The negative of the Shannon entropy derivative is proposed to account for electron density contraction as the chemical bonds are breaking and forming during a chemical reaction. We called this property the electron density contraction index, EDC, which allows identifying stages in a reaction that are dominated by electron contraction or expansion. Four different reactions were analyzed to show how the EDC index changes along the reaction coordinate. The results indicate that the rate of change of Shannon entropy is directly related to the rate of change of the electron density at the bond critical points between all the atomic pairs in the molecular systems. It is expected that EDC will complement the detailed analysis of reaction mechanisms that can be performed with the theoretical tools available to date.
Methods: Density functional theory calculations at the B3LYP/6-31G(d,p) level of theory were carried out using Gaussian 16 to analyze the reaction mechanisms of the four reactions studied. The reaction paths were obtained via the intrinsic reaction coordinate method, which served as the reaction coordinate to obtain the reaction force and the EDC profiles in each case. Shannon entropy and electron density at the bond critical points were calculated using the Multiwfn 3.7 package.
(© 2024. The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.)
Databáze: MEDLINE
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