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Issue 2, 2012
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QM/MM simulation of liquid water with an adaptive quantum region

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Abstract

The simulation of complex chemical systems often requires a multi-level description, in which a region of special interest is treated using a computationally expensive quantum mechanical (QM) model while its environment is described by a faster, simpler molecular mechanical (MM) model. Furthermore, studying dynamic effects in solvated systems or bio-molecules requires a variable definition of the two regions, so that atoms or molecules can be dynamically re-assigned between the QM and MM descriptions during the course of the simulation. Such reassignments pose a problem for traditional QM/MM schemes by exacerbating the errors that stem from switching the model at the boundary. Here we show that stable, long adaptive simulations can be carried out using density functional theory with the BLYP exchange-correlation functional for the QM model and a flexible TIP3P force field for the MM model without requiring adjustments of either. Using a primary benchmark system of pure water, we investigate the convergence of the liquid structure with the size of the QM region, and demonstrate that by using a sufficiently large QM region (with radius 6 Å) it is possible to obtain radial and angular distributions that, in the QM region, match the results of fully quantum mechanical calculations with periodic boundary conditions, and, after a smooth transition, also agree with fully MM calculations in the MM region. The key ingredient is the accurate evaluation of forces in the QM subsystem which we achieve by including an extended buffer region in the QM calculations. We also show that our buffered-force QM/MM scheme is transferable by simulating the solvated Cl ion.

Graphical abstract: QM/MM simulation of liquid water with an adaptive quantum region

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Publication details

The article was received on 12 Aug 2011, accepted on 26 Oct 2011 and first published on 16 Nov 2011


Article type: Paper
DOI: 10.1039/C1CP22600B
Citation: Phys. Chem. Chem. Phys., 2012,14, 646-656
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    QM/MM simulation of liquid water with an adaptive quantum region

    N. Bernstein, C. Várnai, I. Solt, S. A. Winfield, M. C. Payne, I. Simon, M. Fuxreiter and G. Csányi, Phys. Chem. Chem. Phys., 2012, 14, 646
    DOI: 10.1039/C1CP22600B

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