Vapor–liquid equilibrium of water with the MB-pol many-body potential

Muniz, Maria Carolina; Gartner, Thomas E.; Riera, Marc; Knight, Chris; Yue, Shuwen; Paesani, Francesco; Panagiotopoulos, Athanassios Z.

doi:10.1063/5.0050068

Cited by 54 publications

(68 citation statements)

References 53 publications

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“…It should be noted that, since our many-body PEFs directly target the underlying molecular interactions, differences in the representation of the 1-body (1B) term of Eq. ( 5 ) have been found to be negligible for modeling the properties of liquid water 107 and the air/water interface 110 .…”

Section: Methodsmentioning

confidence: 99%

Elevating density functional theory to chemical accuracy for water simulations through a density-corrected many-body formalism

et al. 2021

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Density functional theory (DFT) has been extensively used to model the properties of water. Albeit maintaining a good balance between accuracy and efficiency, no density functional has so far achieved the degree of accuracy necessary to correctly predict the properties of water across the entire phase diagram. Here, we present density-corrected SCAN (DC-SCAN) calculations for water which, minimizing density-driven errors, elevate the accuracy of the SCAN functional to that of “gold standard” coupled-cluster theory. Building upon the accuracy of DC-SCAN within a many-body formalism, we introduce a data-driven many-body potential energy function, MB-SCAN(DC), that quantitatively reproduces coupled cluster reference values for interaction, binding, and individual many-body energies of water clusters. Importantly, molecular dynamics simulations carried out with MB-SCAN(DC) also reproduce the properties of liquid water, which thus demonstrates that MB-SCAN(DC) is effectively the first DFT-based model that correctly describes water from the gas to the liquid phase.

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Section: Methodsmentioning

confidence: 99%

Elevating density functional theory to chemical accuracy for water simulations through a density-corrected many-body formalism

et al. 2021

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“…The 1B, 2B, and 3B terms that involve only the water molecules are described by the MB-pol PEF. [65][66][67] MB-pol has been shown to correctly reproduce the properties of water across all phases, 68,69 including gas-phase clusters [70][71][72][73][74][75][76][77][78][79][80][81] liquid water at ambient conditions [82][83][84][85][86][87][88] and in the supercooled regime, 89 the air/water interface,, [90][91][92][93][94] and various ice phases. [95][96][97][98] The 2B and 3B ion-water terms were fitted to reproduce the corresponding 2B and 3B reference energies that were calculated at the explicitly correlated coupled cluster and canonical cou-pled cluster levels of theory, respectively, including single, double, and perturbative triple excitations, i.e., CCSD(T)-F12b for the 2-body energies, and CCSD(T) for the 3-body energies.…”

Section: Methods Mb-nrg Potential Energy Functionsmentioning

confidence: 99%

Hydration Structure of Na+ and K+ Ions in Solution Predicted by Data-Driven Many-Body Potentials

Zhuang

Riera

Zhou

et al. 2022

Preprint

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The hydration structure of Na+ and K+ ions in solution is systematically investigated using a hierarchy of molecular models that progressively include more accurate representations of many-body interactions. We found that a conventional empirical pairwise additive force field that is commonly used in biomolecular simulations is unable to reproduce the extended X-ray absorption fine structure (EXAFS) spectra for both ions. In contrast, progressive inclusion of many-body effects rigorously derived from the many-body expansion of the energy allows the MB-nrg potential energy functions (PEFs) to achieve nearly quantitative agreement with the experimental EXAFS spectra, thus enabling the development of a molecular-level picture of the hydration structure of both Na+ and K+ in solution. Since the MB-nrg PEFs have already been shown to accurately describe isomeric equilibria and vibrational spectra of small ion–water clusters in the gas phase, the present study demonstrates that the MB-nrg PEFs effectively represent the long-sought-after models able to correctly predict the properties of ionic aqueous systems from the gas to the liquid phase, which has so far remained elusive.

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“…Since the MBE converges quickly for nonmetallic systems, it has been used as a rigorous theoretical framework for the development of several models for various molecular systems. 28,30,36,38,[40][41][42][43][44][45][46][47] Notably, these models have shown remarkable agreement with experimental data for both gas and liquid properties, 30,40,[47][48][49][50][51][52] providing evidence for the transferable nature of the MBE framework.…”

Section: A Many-body Potential Energy Surfacesmentioning

confidence: 81%

Transferability of data-driven, many-body models for CO2 simulations in the vapor and liquid phases

Yue

Riera

Ghosh

et al. 2021

Preprint

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Extending on previous work by Riera et al. [J. Chem. Theory Comput. 16, 2246 (2020)], we introduce a second generation family of data-driven many-body MB-nrg models for CO2 and systematically assess how the strength and anisotropy of the CO2-CO2 interactions affect the models' ability to predict vapor, liquid, and vapor-liquid equilibrium properties. Building upon the many-body expansion formalism, we construct a series of MB-nrg models by fitting 1-body and 2-body reference energies calculated at the coupled cluster level of theory for large monomer and dimer training sets. Advancing from the first generation models, we employ the Charge Model 5 scheme to determine the atomic charges and systematically scale the 2-body energies to obtain more accurate descriptions of vapor, liquid, and vapor-liquid equilibrium properties. Comparisons with the polarizable TTM-nrg model, which is constructed from the same training sets as the MB-nrg models but using a simpler representation of short-range interactions based on conventional Born-Mayer functions, showcase the necessity of high dimensional functional forms for an accurate description of the multidimensional energy landscape of liquid CO2. These findings emphasize the key role played by the training set quality and flexibility of the fitting functions in the development of transferable, data-driven models which, accurately representing high-dimensional many-body effects, can enable predictive computer simulations of molecular fluids across the entire phase diagram.

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Vapor–liquid equilibrium of water with the MB-pol many-body potential

Cited by 54 publications

References 53 publications

Elevating density functional theory to chemical accuracy for water simulations through a density-corrected many-body formalism

Elevating density functional theory to chemical accuracy for water simulations through a density-corrected many-body formalism

Hydration Structure of Na+ and K+ Ions in Solution Predicted by Data-Driven Many-Body Potentials

Transferability of data-driven, many-body models for CO2 simulations in the vapor and liquid phases

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