The influence of polarizability and charge transfer on specific ion effects in the dynamics of aqueous salt solutions

Nguyen, Mary; Rick, Steven W.

doi:10.1063/1.5012682

Cited by 23 publications

(30 citation statements)

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“…This is similar to the inverse power relationship for ions noted by Cheatham 54 and Rick. 55 From the data in Figure 2a,b, D t (0) = 1.090 × 10 −9 m 2 /s and D u (0) = 1.720 × 10 −9 m 2 /s, and from data in Figure 3a Figure S2 in the Supporting Information), which is consistent considering the relative concentrations of solute and solvent. However, the nature of the relationship is not as important as demonstrating that diffusion and hydrogen bond lifetimes are correlated.…”

Section: Resultssupporting

confidence: 79%

Dynamical Effects of Trimethylamine N-Oxide on Aqueous Solutions of Urea

Teng

Ichiye

2019

J. Phys. Chem. B

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Trimethylamine N-oxide (TMAO) stabilizes protein structures, whereas urea destabilizes proteins, and their opposing effects can be counteracted at a 1:2 ratio of TMAO to urea. To investigate how they affect solution dynamics, molecular dynamics simulations have been carried out for aqueous solutions of TMAO and urea at different concentrations. In the binary solutions, urea mainly slows the diffusion of waters that are hydrogen bonded to it (i.e., hydration water), whereas TMAO dramatically slows the diffusion of both hydration water and bulk water because of long-lived TMAO-water hydrogen bonds. In the ternary solutions, because TMAO decreases the diffusion rate of bulk water, the lifetimes of not only water-water but also urea-water hydrogen bonds increase. In addition, the constant forming and breaking of short lifetime hydrogen bonds between urea and water appears to impart energy into the bulk, whereas the long lifetime hydrogen bonds between TMAO and water slows down the bulk, resulting in the compensating effects on bulk water in the ternary solution. This suggests that the counteracting effects of TMAO on urea denaturation may be both to make longer lived hydrogen bonds to water and to counter the energizing effects of urea on bulk water.

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Section: Resultssupporting

confidence: 79%

Dynamical Effects of Trimethylamine N-Oxide on Aqueous Solutions of Urea

Teng

Ichiye

2019

J. Phys. Chem. B

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“…There is also a maximum amount of CT for each pair that is dependent on the distance and decays to zero at large separations in order to limit the unphysical low-energy long-range transfer. 102,106…”

Section: Treatment Of Induced Polarization In MD Simulationsmentioning

confidence: 99%

Molecular Dynamics Simulations of Ionic Liquids and Electrolytes Using Polarizable Force Fields

et al. 2019

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Many applications in chemistry, biology, and energy storage/conversion research rely on molecular simulations to provide fundamental insight into structural and transport properties of materials with high ionic concentrations. Whether the system is comprised entirely of ions, like ionic liquids, or is a mixture of a polar solvent with a salt, e.g., liquid electrolytes for battery applications, the presence of ions in these materials results in strong local electric fields polarizing solvent molecules and large ions. To predict properties of such systems from molecular simulations often requires either explicit or mean-field inclusion of the influence of polarization on electrostatic interactions. In this manuscript, we review the pros and cons of different treatments of polarization ranging from the mean-field approaches to the most popular explicit polarization models in molecular dynamics simulations of ionic materials. For each method, we discuss their advantages and disadvantages and emphasize key assumptions as well as their adjustable parameters. Strategies for the development of polarizable models are presented with a specific focus on extracting atomic polarizabilities. Finally, we compare simulations using polarizable and nonpolarizable models for several classes of ionic systems, discussing the underlying physics that each approach includes or ignores, implications for implementation and computational efficiency, and the accuracy of properties predicted by these methods compared to experiments.

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“…In the following years, a variety of studies have followed suit, combining the JC TIP4P/Ewoptimized ion parameters (JCTIP4PEw) or other ion parameters with the TIP4P/2005 water model. [20][21][22][23][24][25][26][27][28][29][30][31][32][33][34][35][36][37] Following the increased use of TIP4P/2005 and demand of ion parameters specifically optimized for TIP4P/2005, the Vega group started working on obtaining parameters for NaCl in terms of solubility. 41,42 The final parameters are presented in the study of Benavides et al 43 Recently, additional ion parameters were published, 44 for Li + , Na + , K + , Mg 2+ , Ca 2+ , Cl − , and SO 2− 4 .…”

Section: Introductionmentioning

confidence: 99%