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- W2050725147 abstract "Extraction of relaxation times, lifetimes, and rates associated with the transport of topological charge defects in hydrogen-bonded networks from molecular dynamics simulations is a challenge because proton transfer reactions continually change the identity of the defect core. In this paper, we present a statistical mechanical theory that allows these quantities to be computed in an unbiased manner. The theory employs a set of suitably defined indicator or population functions for locating a defect structure and their associated correlation functions. These functions are then used to develop a chemical master equation framework from which the rates and lifetimes can be determined. Furthermore, we develop an integral equation formalism for connecting various types of population correlation functions and derive an iterative solution to the equation, which is given a graphical interpretation. The chemical master equation framework is applied to the problems of both hydronium and hydroxide transport in bulk water. For each case it is shown that the theory establishes direct links between the defect’s dominant solvation structures, the kinetics of charge transfer, and the mechanism of structural diffusion. A detailed analysis is presented for aqueous hydroxide, examining both reorientational time scales and relaxation of the rotational anisotropy, which is correlated with recent experimental results for these quantities. Finally, for OH−(aq) it is demonstrated that the “dynamical hypercoordination mechanism” is consistent with available experimental data while other mechanistic proposals are shown to fail. As a means of going beyond the linear rate theory valid from short up to intermediate time scales, a fractional kinetic model is introduced in the Appendix in order to describe the nonexponential long-time behavior of time-correlation functions. Within the mathematical framework of fractional calculus the power law decay ∼t−σ, where σ is a parameter of the model and depends on the dimensionality of the system, is obtained from Mittag–Leffler functions due to their long-time asymptotics, whereas (stretched) exponential behavior is found for short times." @default.
- W2050725147 created "2016-06-24" @default.
- W2050725147 creator A5055636861 @default.
- W2050725147 creator A5068215051 @default.
- W2050725147 creator A5072717593 @default.
- W2050725147 date "2010-09-28" @default.
- W2050725147 modified "2023-10-18" @default.
- W2050725147 title "A statistical mechanical theory of proton transport kinetics in hydrogen-bonded networks based on population correlation functions with applications to acids and bases" @default.
- W2050725147 cites W1480238028 @default.
- W2050725147 cites W1518556703 @default.
- W2050725147 cites W1527165955 @default.
- W2050725147 cites W1576668315 @default.
- W2050725147 cites W1966108258 @default.
- W2050725147 cites W1969715908 @default.
- W2050725147 cites W1970699034 @default.
- W2050725147 cites W1972310942 @default.
- W2050725147 cites W1973289313 @default.
- W2050725147 cites W1973869488 @default.
- W2050725147 cites W1974358989 @default.
- W2050725147 cites W1974974739 @default.
- W2050725147 cites W1975834451 @default.
- W2050725147 cites W1977446716 @default.
- W2050725147 cites W1978894707 @default.
- W2050725147 cites W1984827804 @default.
- W2050725147 cites W1984869419 @default.
- W2050725147 cites W1987017694 @default.
- W2050725147 cites W1988678591 @default.
- W2050725147 cites W2007387941 @default.
- W2050725147 cites W2007893417 @default.
- W2050725147 cites W2010317468 @default.
- W2050725147 cites W2010499880 @default.
- W2050725147 cites W2013570914 @default.
- W2050725147 cites W2013885842 @default.
- W2050725147 cites W2016585644 @default.
- W2050725147 cites W2019066123 @default.
- W2050725147 cites W2019923586 @default.
- W2050725147 cites W2023271753 @default.
- W2050725147 cites W2024135408 @default.
- W2050725147 cites W2024303155 @default.
- W2050725147 cites W2024891605 @default.
- W2050725147 cites W2025346738 @default.
- W2050725147 cites W2025554319 @default.
- W2050725147 cites W2027356186 @default.
- W2050725147 cites W2027765759 @default.
- W2050725147 cites W2029042254 @default.
- W2050725147 cites W2038935283 @default.
- W2050725147 cites W2039263184 @default.
- W2050725147 cites W2039517674 @default.
- W2050725147 cites W2039962178 @default.
- W2050725147 cites W2041616689 @default.
- W2050725147 cites W2046001409 @default.
- W2050725147 cites W2046608672 @default.
- W2050725147 cites W2049079467 @default.
- W2050725147 cites W2050112352 @default.
- W2050725147 cites W2051638855 @default.
- W2050725147 cites W2054134130 @default.
- W2050725147 cites W2055036655 @default.
- W2050725147 cites W2056821613 @default.
- W2050725147 cites W2058698452 @default.
- W2050725147 cites W2059838064 @default.
- W2050725147 cites W2060855868 @default.
- W2050725147 cites W2062856462 @default.
- W2050725147 cites W2064141166 @default.
- W2050725147 cites W2065329899 @default.
- W2050725147 cites W2067140406 @default.
- W2050725147 cites W2068949508 @default.
- W2050725147 cites W2071954294 @default.
- W2050725147 cites W2071969179 @default.
- W2050725147 cites W2074079785 @default.
- W2050725147 cites W2075935605 @default.
- W2050725147 cites W2078184681 @default.
- W2050725147 cites W2082711435 @default.
- W2050725147 cites W2083454908 @default.
- W2050725147 cites W2084628727 @default.
- W2050725147 cites W2084825573 @default.
- W2050725147 cites W2085061065 @default.
- W2050725147 cites W2086079563 @default.
- W2050725147 cites W2086295275 @default.
- W2050725147 cites W2086957099 @default.
- W2050725147 cites W2088412673 @default.
- W2050725147 cites W2095363688 @default.
- W2050725147 cites W2098235814 @default.
- W2050725147 cites W2099783677 @default.
- W2050725147 cites W2101351503 @default.
- W2050725147 cites W2109671158 @default.
- W2050725147 cites W2111271983 @default.
- W2050725147 cites W2116223045 @default.
- W2050725147 cites W2127400370 @default.
- W2050725147 cites W2127535453 @default.
- W2050725147 cites W2128097747 @default.
- W2050725147 cites W2140506809 @default.
- W2050725147 cites W2141974987 @default.
- W2050725147 cites W2146752617 @default.
- W2050725147 cites W2152414522 @default.
- W2050725147 cites W2159139672 @default.
- W2050725147 cites W2161580626 @default.
- W2050725147 cites W2167154952 @default.
- W2050725147 cites W2169513358 @default.
- W2050725147 cites W2171447759 @default.
- W2050725147 cites W2793463880 @default.