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Ab initio molecular-dynamics simulation of aqueous proton solvation and transport revisited
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10.1063/1.1961443
/content/aip/journal/jcp/123/4/10.1063/1.1961443
http://aip.metastore.ingenta.com/content/aip/journal/jcp/123/4/10.1063/1.1961443
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Figures

Image of FIG. 1.
FIG. 1.

(Color online) Oxygen-oxygen , hydrogen-oxygen , and hydrogen-hydrogen radial distribution functions (RDFs) for water from the CPMD simulations using the BLYP XC functional and fictitious electronic mass of [thin (blue online) solid lines]. The RDFs from CPMD using the BLYP XC functional and a fictitious electronic mass of [thick gray (cyan online) solid lines] and from recent neutron-diffraction experiments by Soper (Ref. 30) [dashed (green online) lines] are shown for comparison.

Image of FIG. 2.
FIG. 2.

(Color online) RDFs for water from the CPMD simulations using the HCTH XC functional and fictitious electronic mass of [thin (blue online) solid lines]. The RDFs from CPMD using the BLYP XC functional and a fictitious electronic mass of [thick gray (cyan online) solid lines] and from recent neutron-diffraction experiments by Soper (Ref. 30) [dashed (green online) lines] are shown for comparison.

Image of FIG. 3.
FIG. 3.

Mean-square displacement (MSD), , of molecular water oxygen from the same CPMD simulations as in Figs. 1 and 2.

Image of FIG. 4.
FIG. 4.

(Color online) The water-hydronium RDF from CPMD simulations using the BLYP [gray (cyan online) line] and HCTH [thick solid (black online) line] XC functionals. The for the BLYP simulations from Fig. 1 and for the HCTH simulation from Fig. 2 are shown for comparison, respectively, in dashed and solid thin (green online) lines.

Image of FIG. 5.
FIG. 5.

Index of the oxygen atom carrying the excess proton as a function of time. Panel (a): BLYP (I), Panel (b): BLYP (II), and Panel (c): HCTH CPMD simulations. For the BLYP simulations the index of the special oxygen to which the excess proton is preferably associated is marked (dashed horizontal lines).

Image of FIG. 6.
FIG. 6.

Mean-square displacements (MSDs), , of the hydronium oxygen (thick solid lines) and water oxygen (thin solid lines) from the same simulations as in Fig. 5. For BLYP simulations [panels (a) and (b)] MSDs of the special oxygen to which the excess proton is preferably associated in the simulation are shown (dashed lines). For the BLYP (II) simulation two graphs which differ by scale in the vertical direction are presented. The straight dotted line is the least-squares linear approximation to the diffusive part of the MSD function used to evaluate the excess proton diffusion coefficient.

Image of FIG. 7.
FIG. 7.

Histograms of the distribution of the number of back and forth proton-transfer events within the same special bond (upper parts of the panels) and of the hops when the excess proton was associated with three different water molecules during each two subsequent hops (low parts of the panels) as functions of the time interval between the two subsequent hops. Panel (a): BLYP (I), Panel (b): BLYP (II), and Panel (c): HCTH CPMD simulations.

Image of FIG. 8.
FIG. 8.

Cumulative lifetime of the special bond [see Eq. (1)] in the simulation as a function of the largest time separating two subsequent proton-transfer events between oxygen forming the special bond as calculated from the data shown in Fig. 7. The thick line for reoccurring “Zundel” jumps and the thin line for forest (“Eigen”) jumps.

Image of FIG. 9.
FIG. 9.

(Color online) Distribution function of the proton-transfer coordinate [Eq. (2)]. The dashed (blue online) curve is the distribution of the reoccurring proton-transfer events within (i.e., when the Zundel complex is prevailing) and the thin solid (red online) curve is the distribution of the remaining of proton-transfer events (i.e., when the eigencomplex is prevailing). The thick solid (black online) line is the total distribution . Panel (a): BLYP (II) simulation, Panel (b): HCTH simulation.

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/content/aip/journal/jcp/123/4/10.1063/1.1961443
2005-08-02
2014-04-20
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Ab initio molecular-dynamics simulation of aqueous proton solvation and transport revisited
http://aip.metastore.ingenta.com/content/aip/journal/jcp/123/4/10.1063/1.1961443
10.1063/1.1961443
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