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Multiscale reactive molecular dynamics
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10.1063/1.4743958
/content/aip/journal/jcp/137/22/10.1063/1.4743958
http://aip.metastore.ingenta.com/content/aip/journal/jcp/137/22/10.1063/1.4743958

Figures

Image of FIG. 1.
FIG. 1.

Example of the reactive complexes formed for the (a) excess proton and (b) hydroxide ion. The dashed line indicates the boundary between those atoms within the reactive complex and the rest of the system, which dynamically changes over the course of a simulation.

Image of FIG. 2.
FIG. 2.

Pairwise potentials (solid lines) and forces (dashed lines) from the B-spline fits for hydronium-water interactions plotted as a function of interatomic separation. The atom labels are defined in the text.

Image of FIG. 3.
FIG. 3.

Flow chart outlining the iterative force-matching algorithm used to develop reactive models.

Image of FIG. 4.
FIG. 4.

Tabulated potentials (solid lines) and forces (dashed) for diabatic corrections (a) , (b) in Eq. (6) and off-diagonal geometric factor (c) A GEO in Eq. (2) for the excess proton (black) and hydroxide ion (red) reactive models.

Image of FIG. 5.
FIG. 5.

Probability distributions for the hydroxide water-oxygen angle (HH–OH–OW) for the AIMD simulation (solid lines) and FM-based MS-RMD models (dashed lines). The full distribution (black) is decomposed into contributions from solvation structures with three (red), four (green), and five (blue) water molecules donating H-bonds to the hydroxide ion, with relative populations indicated.

Image of FIG. 6.
FIG. 6.

Radial distribution functions (solid lines) and integrated coordination numbers (dashed lines) between atoms of the hydronium cation and water molecules. For each plot, results from the AIMD (black), nonreactive (blue), and reactive MS-RMD (red) models are shown. The atom labels are defined in the text.

Image of FIG. 7.
FIG. 7.

Potentials of mean force along a proton transfer coordinate for the excess proton and hydroxide models. Results are shown for the AIMD (solid black), nonreactive (dashed blue), and reactive (dot-dashed red) models.

Image of FIG. 8.
FIG. 8.

Radial distribution functions (solid lines) and integrated coordination numbers (dashed lines) between atoms of the hydroxide ion and water molecules. For each plot, results from the AIMD (black), nonreactive (blue), and reactive MS-RMD (red) models are shown. The atom labels are defined in the text.

Tables

Generic image for table
Table I.

B-spline coefficients for each hydronium-water interatomic pair in the nonreactive model. The values of r core used in the B-spline fits are 2.0, 1.2, 0.9, and 1.2 Å for the OH–OW, OH–HW, HH–OW, and HH–HW interatomic pairs, respectively. The evenly spaced bin widths for the corresponding curves were 0.58, 0.33, 0.23, and 0.33 Å. The value of r cut remained at 7.8 Å and a polynomial order of 6 was used for all curves. Trailing zeroed coefficients for each curve are omitted for clarity, and the resulting curves are shown in Fig. 2.

Generic image for table
Table II.

B-spline coefficients for the diabatic corrections and off-diagonal geometric factor for the reactive excess proton model. The values of r core used in the B-spline fits are 2.0, 0.8, and 2.1 Å for the , , and A GEO interactions, respectively. The evenly spaced bin widths for the corresponding curves were 0.085, 0.045, and 0.0525 Å. The value of r cut was 2.85, 1.25, and 3.15 Å for the corresponding curves, and a polynomial order of 6 was used for all curves. Trailing zeroed coefficients for each curve are omitted for clarity, and the resulting curves are shown in Fig. 4.

Generic image for table
Table III.

Optimized model parameters for the off-diagonal couplings for FM reactive proton and hydroxide models.

Generic image for table
Table IV.

B-spline coefficients for the diabatic corrections and off-diagonal geometric factor for the reactive hydroxide model. The values of r core used in the B-spline fits are 2.0, 0.9, and 2.3 Å for , , and A GEO interactions, respectively. The evenly spaced bin widths for the corresponding curves were 0.085, 0.035, and 0.085 Å. The value of r cut was 2.85, 1.25, and 3.15 Å for the corresponding curves and a polynomial order of 6 was used for all curves. Trailing zeroed coefficients for each curve are omitted for clarity and the resulting curves are shown in Fig. 4.

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/content/aip/journal/jcp/137/22/10.1063/1.4743958
2012-08-15
2014-04-17
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Multiscale reactive molecular dynamics
http://aip.metastore.ingenta.com/content/aip/journal/jcp/137/22/10.1063/1.4743958
10.1063/1.4743958
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