Chemical Accuracy in Modeling Halide Ion Hydration from Many-Body Representations

Paesani, Francesco; Bajaj, Pushp; Riera, Marc

doi:10.26434/chemrxiv.6789326

Cited by 15 publications

(19 citation statements)

References 118 publications

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“…Many-body reference energies, calculated using the SAMBA approach, 122 are listed in Tables 1 and 2 we found to consistently provide good agreement with coupled-cluster reference energies for various aqueous and non-aqueous systems. 83,85,86,96,97,128,129 As expected from the correlation plots shown in Fig. 2, the TTM-nrg PEF displays significantly larger deviations from the ref- Table 2 for individual terms of the MBE in Eq.1 calculated at the ωB97M-V, TTM-nrg, and MB-nrg levels of theory for the same (CH 4 ) m (H 2 O) n clusters, with m + n ≤ 5, shown in Fig.3.…”

Section: Assessment Of Ttm-nrg and Mb-nrg Accuracysupporting

confidence: 55%

“…1 to develop TTM-nrg and MB-nrg PEFs for halide-water, 82,83 alkali-metal ion-water, 84,85 and carbon dioxide-water systems, 86 which have been employed in computer simulations of various aqueous systems. [94][95][96][97][98][99][100][101] While both TTM-nrg and MB-nrg PEFs rely on MB-pol to describe water-water interactions, they differ in the functional forms adopted to represent solute distortions and solute-water interactions. In the TTM-nrg PEF, the CH 4 1B term is represented by a functional form similar to those used in common force fields, which is expressed in Eq.…”

Section: Ttm-nrg and Mb-nrg Functional Formsmentioning

confidence: 99%

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Data-Driven Many-Body Models with Chemical Accuracy for CH4/H2O Mixtures

Riera¹,

Hirales²,

Ghosh³

et al. 2020

Preprint

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<div> <div> <div> <p>Many-body potential energy functions (PEFs) based on the TTM-nrg and MB-nrg theoretical/computational frameworks are developed from coupled cluster reference data for neat methane and mixed methane/water systems. It is shown that that the MB-nrg PEFs achieve subchemical accuracy in the representation of individual many-body effects in small clusters and enables predictive simulations from the gas to the liquid phase. Analysis of structural properties calculated from molecular dynamics simulations of liquid methane and methane/water mixtures using both TTM-nrg and MB-nrg PEFs indicates that, while accounting for polarization effects is important for a correct description of many-body interactions in the liquid phase, an accurate representation of short-range interactions, as provided by the MB-nrg PEFs, is necessary for a quantitative description of the local solvation structure in liquid mixtures. </p> </div> </div> </div>

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Section: Assessment Of Ttm-nrg and Mb-nrg Accuracysupporting

confidence: 55%

Section: Ttm-nrg and Mb-nrg Functional Formsmentioning

confidence: 99%

Data-Driven Many-Body Models with Chemical Accuracy for CH4/H2O Mixtures

Riera¹,

Hirales²,

Ghosh³

et al. 2020

Preprint

Self Cite

View full text Add to dashboard Cite

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“…It should be noted that our previous analyses showed that, among the existing functionals, ωB97M-V consistently provides the closer agreement with CCSD(T) reference data for molecular interactions in aqueous systems. 69,71,81,82,111 As expected from the analysis of the correlation plots in Fig. 2 A direct probe of the multidimensional 2B energy landscape is provided by the second virial coefficient,…”

Section: Many-body Decompositionmentioning

confidence: 67%

“…1 can be correctly represented in terms of classical many-body polarization as described in Section 2.1. In this context, it should be noted that previous studies of manybody effects in aqueous systems indicated that an explicit representation of 3B energies is necessary to guarantee an accurate description of structural, thermodynamic, dynamical and spectroscopic properties of water 75,[109][110][111] as well as halide-water 69,79,[81][82][83][84][85] and alkali-metal ion-water 71,80,86 interactions in the gas phase and in solution. In particular, it was found that significant error cancellation between different terms of the MBE affects the performance of common force fields and DFT models for water.…”

Section: Many-body Decompositionmentioning

confidence: 99%

Data-Driven Many-Body Models for Molecular Fluids: CO₂/H₂O Mixtures as a Case Study

Riera

Yeh

Paesani

2020

J. Chem. Theory Comput.

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In this study, we extend the scope of the many-body TTM-nrg and MB-nrg potential energy functions (PEFs), originally introduced for halide ion-water and alkali-metal ion-water interactions, to the modeling of carbon dioxide (CO 2) and water (H 2 O) mixtures as prototypical examples of molecular fluids. Both TTM-nrg and MB-nrg PEFs are derived entirely from electronic structure data obtained at the coupled cluster level of theory and are, by construction, compatible with MB-pol, a many-body PEF that has been shown to accurately reproduce the properties of water. Although both TTM-nrg and MB-nrg PEFs adopt the same functional forms for describing permanent electrostatics, polarization, and dispersion, they differ in the representation of short-range contributions, with the TTM-nrg PEFs relying on conventional Born-Mayer expressions and the MB-nrg PEFs employing multidimensional permutationally invariant polynomials. By providing a physically correct description of many-body effects at both short and long ranges, the MB-nrg PEFs are shown to quantitatively represent the global potential energy surfaces of the CO 2-CO 2 and CO 2-H 2 O dimers and the energetics of small clusters as well as to correctly reproduce various properties in both gas and liquid phases. Building upon previous studies of aqueous systems, our analysis provides further evidence for the accuracy and efficiency of the MB-nrg framework in representing molecular interactions in fluid mixtures at different temperature and pressure conditions. File list (3) download file view on ChemRxiv many-body_mixtures.pdf (3.97 MiB) download file view on ChemRxiv supp_info.pdf (151.39 KiB) download file view on ChemRxiv co2_h2o.pdf (266.17 KiB)

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“…Many of these models, while yielding very accurate results, are computationally expensive. For example, MB-pol is regarded as one of the most accurate models, but it is ∼50 times more computationally expensive than AMOEBA, and has not yet been used for simulations beyond water 133 − 136 and water-halide (using MB-nrg which is based on MB-pol 137 ) systems. For further information about advanced water models, including parametrization and machine learning methods, the reader is directed to the recent review papers by Cisneros et al.…”

Section: Water Models In Molecular Dynamics Simulationsmentioning

confidence: 99%

Water in Nanopores and Biological Channels: A Molecular Simulation Perspective

2020

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This Review explores the dynamic behavior of water within nanopores and biological channels in lipid bilayer membranes. We focus on molecular simulation studies, alongside selected structural and other experimental investigations. Structures of biological nanopores and channels are reviewed, emphasizing those high-resolution crystal structures, which reveal water molecules within the transmembrane pores, which can be used to aid the interpretation of simulation studies. Different levels of molecular simulations of water within nanopores are described, with a focus on molecular dynamics (MD). In particular, models of water for MD simulations are discussed in detail to provide an evaluation of their use in simulations of water in nanopores. Simulation studies of the behavior of water in idealized models of nanopores have revealed aspects of the organization and dynamics of nanoconfined water, including wetting/dewetting in narrow hydrophobic nanopores. A survey of simulation studies in a range of nonbiological nanopores is presented, including carbon nanotubes, synthetic nanopores, model peptide nanopores, track-etched nanopores in polymer membranes, and hydroxylated and functionalized nanoporous silica. These reveal a complex relationship between pore size/geometry, the nature of the pore lining, and rates of water transport. Wider nanopores with hydrophobic linings favor water flow whereas narrower hydrophobic pores may show dewetting. Simulation studies over the past decade of the behavior of water in a range of biological nanopores are described, including porins and β-barrel protein nanopores, aquaporins and related polar solute pores, and a number of different classes of ion channels. Water is shown to play a key role in proton transport in biological channels and in hydrophobic gating of ion channels. An overall picture emerges, whereby the behavior of water in a nanopore may be predicted as a function of its hydrophobicity and radius. This informs our understanding of the functions of diverse channel structures and will aid the design of novel nanopores. Thus, our current level of understanding allows for the design of a nanopore which promotes wetting over dewetting or vice versa. However, to design a novel nanopore, which enables fast, selective, and gated flow of water de novo would remain challenging, suggesting a need for further detailed simulations alongside experimental evaluation of more complex nanopore systems.

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Chemical Accuracy in Modeling Halide Ion Hydration from Many-Body Representations

Cited by 15 publications

References 118 publications

Data-Driven Many-Body Models with Chemical Accuracy for CH4/H2O Mixtures

Data-Driven Many-Body Models with Chemical Accuracy for CH4/H2O Mixtures

Data-Driven Many-Body Models for Molecular Fluids: CO₂/H₂O Mixtures as a Case Study

Water in Nanopores and Biological Channels: A Molecular Simulation Perspective

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Chemical Accuracy in Modeling Halide Ion Hydration from Many-Body Representations

Cited by 15 publications

References 118 publications

Data-Driven Many-Body Models with Chemical Accuracy for CH4/H2O Mixtures

Data-Driven Many-Body Models with Chemical Accuracy for CH4/H2O Mixtures

Data-Driven Many-Body Models for Molecular Fluids: CO2/H2O Mixtures as a Case Study

Water in Nanopores and Biological Channels: A Molecular Simulation Perspective

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Product

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Data-Driven Many-Body Models for Molecular Fluids: CO₂/H₂O Mixtures as a Case Study