Development of the Quantum Inspired SIBFA Many-Body Polarizable Force Field: Enabling Condensed Phase Molecular Dynamics Simulations. - Archive ouverte HAL Access content directly
Journal Articles Journal of Chemical Theory and Computation Year : 2022

Development of the Quantum Inspired SIBFA Many-Body Polarizable Force Field: Enabling Condensed Phase Molecular Dynamics Simulations.

Abstract

We present the extension of the SIBFA (Sum of Interactions Between Fragments Ab initio Computed) many-body polarizable force field to condensed phase Molecular Dynamics (MD) simulations. The Quantum-Inspired SIBFA procedure is grounded on simplified integrals obtained from localized molecular orbital theory and achieves full separability of its intermolecular potential. It embodies long-range multipolar electrostatics (up to quadrupole) coupled to a short-range penetration correction (up to charge-quadrupole), exchange-repulsion, many-body polarization, many-body charge transfer/delocalization, exchange-dispersion and dispersion (up to C10). This enables the reproduction of all energy contributions of ab initio Symmetry-Adapted Perturbation Theory SAPT(DFT) gas phase reference computations. The SIBFA approach has been integrated within the Tinker-HP massively parallel MD package with all its energy gradients. This novel implementation also notably includes a computationally tractable simplification of the many-body charge transfer/delocalization contribution. As a proof of concept, we perform a first computational experiment defining a water model fitted on a limited set of SAPT(DFT) data. SIBFA is shown to enable a satisfactory reproduction of both gas phase energetic contributions and condensed phase properties highlighting the importance of its physically-motivated functional form.

Dates and versions

hal-03508892 , version 1 (03-01-2022)

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S. Naseem Kahn, L. Lagardère, C. Narth, G. A. Cisneros, P. Ren, et al.. Development of the Quantum Inspired SIBFA Many-Body Polarizable Force Field: Enabling Condensed Phase Molecular Dynamics Simulations.. Journal of Chemical Theory and Computation, 2022, 18 (6), pp.3607-3621. ⟨10.1021/acs.jctc.2c00029⟩. ⟨hal-03508892⟩
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