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

2020 ◽  
Author(s):  
Marc Riera ◽  
Alan Hirales ◽  
Raja Ghosh ◽  
Francesco Paesani
Keyword(s):  
Liquid Phase ◽  
Quantitative Description ◽  
Liquid Mixtures ◽  
Many Body ◽  
Energy Functions ◽  
Potential Energy Functions ◽  
Dynamics Simulations ◽  
Body Potential ◽  
Small Clusters ◽  
Many Body Interactions

<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>

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

2020 ◽  
Author(s):  
Marc Riera ◽  
Alan Hirales ◽  
Raja Ghosh ◽  
Francesco Paesani
Keyword(s):  
Liquid Phase ◽  
Quantitative Description ◽  
Liquid Mixtures ◽  
Many Body ◽  
Energy Functions ◽  
Potential Energy Functions ◽  
Dynamics Simulations ◽  
Body Potential ◽  
Small Clusters ◽  
Many Body Interactions

<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>

Halide Ion Micro-Hydration: Structure, Energetics, and Spectroscopy of Small Halide–Water Clusters

2019 ◽  
Author(s):  
Pushp Bajaj ◽  
Marc Riera ◽  
Jason K. Lin ◽  
Yaira E. Mendoza Montijo ◽  
Jessica Gazca ◽  
...  
Keyword(s):  
Water Clusters ◽  
Quantitative Description ◽  
Three Dimensional ◽  
Many Body ◽  
Ion Hydration ◽  
Potential Energy Functions ◽  
Hydrogen Bond Networks ◽  
Correct Representation ◽  
Dynamics Simulations ◽  
Body Potential

<div> <div> <div> <p>Replica exchange molecular dynamics simulations and vibrational spectroscopy calculations are performed using halide-water many-body potential energy functions to provide a bottom-up analysis of the structures, energetics, and hydrogen-bonding arrangements in X−(H2O)n=3−6 clusters, with X = F, Cl, Br, and I. Independently of the cluster size, it is found that all four halides prefer surface-type structures in which they occupy one of the vertices in the underlying three-dimensional hydrogen-bond networks. For fluoride-water clusters, this is in contrast with previous reports suggesting that fluoride prefers interior-type arrangements, where the ion is fully hydrated. These differences can be ascribed to the variability in how various molecular models are capable to reproduce the subtle interplay between halide-water and water-water interactions. Our results thus emphasize the importance of a correct representation of individual many-body contributions to the molecular interactions for a quantitative description of halide ion hydration. </p> </div> </div> </div>

Halide Ion Micro-Hydration: Structure, Energetics, and Spectroscopy of Small Halide–Water Clusters

2019 ◽  
Author(s):  
Pushp Bajaj ◽  
Marc Riera ◽  
Jason K. Lin ◽  
Yaira E. Mendoza Montijo ◽  
Jessica Gazca ◽  
...  
Keyword(s):  
Water Clusters ◽  
Quantitative Description ◽  
Three Dimensional ◽  
Many Body ◽  
Ion Hydration ◽  
Potential Energy Functions ◽  
Hydrogen Bond Networks ◽  
Correct Representation ◽  
Dynamics Simulations ◽  
Body Potential

<div> <div> <div> <p>Replica exchange molecular dynamics simulations and vibrational spectroscopy calculations are performed using halide-water many-body potential energy functions to provide a bottom-up analysis of the structures, energetics, and hydrogen-bonding arrangements in X−(H2O)n=3−6 clusters, with X = F, Cl, Br, and I. Independently of the cluster size, it is found that all four halides prefer surface-type structures in which they occupy one of the vertices in the underlying three-dimensional hydrogen-bond networks. For fluoride-water clusters, this is in contrast with previous reports suggesting that fluoride prefers interior-type arrangements, where the ion is fully hydrated. These differences can be ascribed to the variability in how various molecular models are capable to reproduce the subtle interplay between halide-water and water-water interactions. Our results thus emphasize the importance of a correct representation of individual many-body contributions to the molecular interactions for a quantitative description of halide ion hydration. </p> </div> </div> </div>

Empirical many-body potential energy functions for iron

1993 ◽  
Vol 97 (46) ◽  
pp. 12073-12082 ◽  
Author(s):  
Fei Gao ◽  
Roy L. Johnston ◽  
John N. Murrell
Keyword(s):  
Potential Energy ◽  
Many Body ◽  
Energy Functions ◽  
Potential Energy Functions ◽  
Body Potential

scholarly journals Infrared Signatures of Isomer Selectivity and Symmetry Breaking in the Cs+(H2O)3 Complex Using Many-Body Potential Energy Functions

2020 ◽  
Author(s):  
Marc Riera ◽  
Justin J. Talbot ◽  
Ryan P. Steele ◽  
Francesco Paesani
Keyword(s):  
Potential Energy ◽  
Potential Energy Surface ◽  
Energy Surface ◽  
Water Clusters ◽  
Quantitative Description ◽  
Experimental Spectrum ◽  
Many Body ◽  
Energy Functions ◽  
Potential Energy Functions ◽  
Three Body

<div> <div> <div> <p>A quantitative description of the interactions between ions and water is key to characterizing the role played by ions in mediating fundamental processes that take place in aqueous environments. At the molecular level, vibrational spectroscopy provides a unique means to probe the multidimensional potential energy surface of small ion−water clusters. In this study, we combine the MB-nrg potential energy functions recently developed for ion−water interactions with perturbative corrections to vibrational self-consistent field theory and the local-monomer approximation to disentangle many-body effects on the stability and vibrational structure of the Cs+(H2O)3 cluster. Since several low-energy, thermodynamically accessible isomers exist for Cs+(H2O)3, even small changes in the description of the underlying potential energy surface can result in large differences in the relative stability of the various isomers. Our analysis demonstrates that a quantitative account for three-body energies and explicit treatment of cross-monomer vibrational couplings are required to reproduce the experimental spectrum. </p> </div> </div> </div>

MB-Fit: Software infrastructure for data-driven many-body potential energy functions

2021 ◽  
Vol 155 (12) ◽  
pp. 124801
Author(s):  
Ethan F. Bull-Vulpe ◽  
Marc Riera ◽  
Andreas W. Götz ◽  
Francesco Paesani
Keyword(s):  
Potential Energy ◽  
Data Driven ◽  
Many Body ◽  
Software Infrastructure ◽  
Energy Functions ◽  
Potential Energy Functions ◽  
Body Potential

Infrared Signatures of Isomer Selectivity and Symmetry Breaking in the Cs+(H2O)3 Complex Using Many-Body Potential Energy Functions

2020 ◽  
Author(s):  
Marc Riera ◽  
Justin J. Talbot ◽  
Ryan P. Steele ◽  
Francesco Paesani
Keyword(s):  
Potential Energy ◽  
Potential Energy Surface ◽  
Energy Surface ◽  
Water Clusters ◽  
Quantitative Description ◽  
Experimental Spectrum ◽  
Many Body ◽  
Energy Functions ◽  
Potential Energy Functions ◽  
Three Body

<div> <div> <div> <p>A quantitative description of the interactions between ions and water is key to characterizing the role played by ions in mediating fundamental processes that take place in aqueous environments. At the molecular level, vibrational spectroscopy provides a unique means to probe the multidimensional potential energy surface of small ion−water clusters. In this study, we combine the MB-nrg potential energy functions recently developed for ion−water interactions with perturbative corrections to vibrational self-consistent field theory and the local-monomer approximation to disentangle many-body effects on the stability and vibrational structure of the Cs+(H2O)3 cluster. Since several low-energy, thermodynamically accessible isomers exist for Cs+(H2O)3, even small changes in the description of the underlying potential energy surface can result in large differences in the relative stability of the various isomers. Our analysis demonstrates that a quantitative account for three-body energies and explicit treatment of cross-monomer vibrational couplings are required to reproduce the experimental spectrum. </p> </div> </div> </div>

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