Ab Initio Molecular Dynamics and Lattice Dynamics-Based Force Field for Modeling Hexagonal Boron Nitride in Mechanical and Interfacial Applications

The speciation of calcium carbonate in water is important to the geochemistry of the world’s oceans and has ignited significant debate regarding the mechanism by which nucleation occurs. Here it is vital to be able to quantify the thermodynamics of ion pairing versus higher order association processes in order to distinguish between possible pathways. Given that it is experimentally challenging to quantify such species, here we determine the thermodynamics for ion pairing and multiple binding of calcium carbonate species using bias-enhanced molecular dynamics. In order to examine the uncertainties underlying these results, we have derived a new polarizable force field for both calcium carbonate and bicarbonate in water based on the AMOEBA model to compare against our earlier rigid-ion model, both of which are further benchmarked against ab initio molecular dynamics for the ion pair. Both force fields consistently indicate that the association of calcium carbonate ion pairs is stable, though with an equilibrium constant that is lower than for ion pairing itself.

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A new universal force-field for the Li2S-P2S5 system

Physical Chemistry Chemical Physics ◽

10.1039/d1cp05393k ◽

2022 ◽

Author(s):

Shunsuke Ariga ◽

Takahiro Ohkubo ◽

Shingo Urata ◽

Yutaka Imamura ◽

Taketoshi Taniguchi

Keyword(s):

Molecular Dynamics ◽

Solid State ◽

Force Field ◽

Ab Initio ◽

Promising Material ◽

Ab Initio Molecular Dynamics ◽

Conduction Mechanisms ◽

Universal Force Field ◽

Solid State Batteries ◽

All Solid State Batteries

Lithium thiophosphate electrolyte is a promising material for application in all-solid-state batteries. Ab initio molecular dynamics (AIMD) simulations have been used to investigate the ion conduction mechanisms in single-crystalline and...

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Calcium ions in aqueous solutions: Accurate force field description aided by ab initio molecular dynamics and neutron scattering

The Journal of Chemical Physics ◽

10.1063/1.5006779 ◽

2018 ◽

Vol 148 (22) ◽

pp. 222813 ◽

Cited By ~ 34

Author(s):

Tomas Martinek ◽

Elise Duboué-Dijon ◽

Štěpán Timr ◽

Philip E. Mason ◽

Katarina Baxová ◽

...

Keyword(s):

Molecular Dynamics ◽

Aqueous Solutions ◽

Force Field ◽

Neutron Scattering ◽

Ab Initio ◽

Calcium Ions ◽

Ab Initio Molecular Dynamics

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Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics

10.26434/chemrxiv.11879805.v1 ◽

2020 ◽

Author(s):

Paolo Raiteri ◽

Alicia Schuitemaker ◽

Julian Gale

Keyword(s):

Molecular Dynamics ◽

Calcium Carbonate ◽

Force Field ◽

Ab Initio ◽

Ion Pairs ◽

Ion Pairing ◽

Ab Initio Molecular Dynamics ◽

Carbonate Solutions ◽

Multiple Binding ◽

Carbonate Species

The speciation of calcium carbonate in water is important to the geochemistry of the world’s oceans and has ignited significant debate regarding the mechanism by which nucleation occurs. Here it is vital to be able to quantify the thermodynamics of ion pairing versus higher order association processes in order to distinguish between possible pathways. Given that it is experimentally challenging to quantify such species, here we determine the thermodynamics for ion pairing and multiple binding of calcium carbonate species using bias-enhanced molecular dynamics. In order to examine the uncertainties underlying these results, we have derived a new polarizable force field for both calcium carbonate and bicarbonate in water based on the AMOEBA model to compare against our earlier rigid-ion model, both of which are further benchmarked against ab initio molecular dynamics for the ion pair. Both force fields consistently indicate that the association of calcium carbonate ion pairs is stable, though with an equilibrium constant that is lower than for ion pairing itself.

Download Full-text