Mutually polarizable QM/MM model with in situ optimized localized basis functions

The Journal of Chemical Physics
Jacek DziedzicChris-Kriton Skylaris

Abstract

We extend our recently developed quantum-mechanical/molecular mechanics (QM/MM) approach [Dziedzic et al., J. Chem. Phys. 145, 124106 (2016)] to enable in situ optimization of the localized orbitals. The quantum subsystem is described with onetep linear-scaling density functional theory and the classical subsystem - with the AMOEBA polarizable force field. The two subsystems interact via multipolar electrostatics and are fully mutually polarizable. A total energy minimization scheme is employed for the Hamiltonian of the coupled QM/MM system. We demonstrate that, compared to simpler models using fixed basis sets, the additional flexibility offered by in situ optimized basis functions improves the accuracy of the QM/MM interface, but also poses new challenges, making the QM subsystem more prone to overpolarization and unphysical charge transfer due to increased charge penetration. We show how these issues can be efficiently solved by replacing the classical repulsive van der Waals term for QM/MM interactions with an interaction of the electronic density with a fixed, repulsive MM potential that mimics Pauli repulsion, together with a modest increase in the damping of QM/MM polarization. We validate our method, with particular at...Continue Reading

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Citations

May 10, 2020·The Journal of Chemical Physics·Joseph C A PrenticeChris-Kriton Skylaris
Aug 28, 2020·Physical Chemistry Chemical Physics : PCCP·Michele NottoliFilippo Lipparini
Aug 10, 2021·Journal of Chemical Theory and Computation·Eleftherios LambrosFrancesco Paesani
Nov 21, 2020·Journal of Chemical Theory and Computation·Eleftherios LambrosFrancesco Paesani
Nov 7, 2019·Journal of Chemical Theory and Computation·Elvar Örn JónssonHannes Jónsson
Aug 10, 2021·Wiley Interdisciplinary Reviews. Computational Molecular Science·Jorge NochebuenaG Andrés Cisneros
Apr 17, 2020·Journal of Chemical Information and Modeling·Richard T BradshawJonathan W Essex
Sep 14, 2019·Journal of Chemical Theory and Computation·Danil S KaliakinSergey A Varganov
Jul 28, 2019·Journal of Chemical Theory and Computation·Filippo Lipparini
Aug 14, 2020·Journal of Chemical Theory and Computation·Claudia I Viquez Rojas, Lyudmila V Slipchenko

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