Journal
JOURNAL OF COMPUTATIONAL CHEMISTRY
Volume 38, Issue 22, Pages 1897-1920Publisher
WILEY
DOI: 10.1002/jcc.24830
Keywords
molecular mechanics; polarizable force field; quantum chemistry; metalloproteins
Categories
Funding
- Grand Equipement National de Calcul Intensif (GENCI)
- Institut du Developpement et des Ressources en Informatique Scientifique (IDRIS)
- Centre Informatique de l'Enseignement Superieur (CINES, France) [x2009-075009]
- Centre de Ressources Informatiques de Haute Normandie (CRIHAN, Rouen, France) [1998053]
- Research Council of Saint-Joseph University of Beirut, Lebanon [FS71]
- Agence Nationale de la Recherche [ANR-14-CE16-0028-01]
- Lebanese National Council for Scientific Research, CNRS-L [FS80]
- French Institute-Campus France au Liban
- French-Lebanese program CEDRE [FS30]
- Agence Nationale de la Recherche (ANR) [ANR-14-CE16-0028] Funding Source: Agence Nationale de la Recherche (ANR)
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A correct representation of the short-range contributions such as exchange-repulsion (E-rep) and charge-transfer (Ect) is essential for the soundness of separable, anisotropic polarizable molecular mechanics potentials. Within the context of the SIBFA procedure, this is aimed at by explicit representations of lone pairs in their expressions. It is necessary to account for their anisotropic behaviors upon performing not only in-plane, but also out-of-plane, variations of a probe molecule or cation interacting with a target molecule or molecular fragment. Thus, Erep and Ect have to reproduce satisfactorily the corresponding anisotropies of their quantum chemical (QC) counterparts. A significant improvement of the out-of-plane dependencies was enabled when the sp(2) and sp localized lone-pairs are, even though to a limited extent, delocalized on both sides of the plane, above and below the atom bearer but at the closely similar angles as the in-plane lone pair. We report calibration and validation tests on a series of monoligated complexes of a probe Zn(II) cation with several biochemically relevant ligands. Validations are then performed on several polyligated Zn(II) complexes found in the recognition sites of Zn-metalloproteins. Such calibrations and validations are extended to representative monoligated and polyligated complexes of Mg(II) and Ca(II). It is emphasized that the calibration of all three cations was for each DE contribution done on a small training set bearing on a limited number of representative N-, O-, and S- monoligated complexes. Owing to the separable nature of DE, a secure transferability is enabled to a diversity of polyligated complexes. For these the relative errors with respect to the target DE(QC) values are generally< 3%. Overall, the article proposes a full set of benchmarks that could be useful for force field developers. (C) 2017 Wiley Periodicals, Inc.
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