Extending on the previous work by Riera et al. [J. Chem. Theory Comput. 16, 2246–2257 (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 one-body and two-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 two-body energies to obtain more accurate descriptions of vapor, liquid, and vapor–liquid equilibrium properties. Challenges in model construction arise due to the anisotropic nature and small magnitude of the interaction energies in CO2, calling for the necessity of highly accurate descriptions of the multidimensional energy landscape of liquid CO2. These findings emphasize the key role played by the training set quality 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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14 March 2022
Research Article|
March 09 2022
Transferability of data-driven, many-body models for CO2 simulations in the vapor and liquid phases
Shuwen Yue
;
Shuwen Yue
1
Department of Chemical and Biological Engineering, Princeton University
, Princeton, New Jersey 08544, USA
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Marc Riera
;
Marc Riera
2
Department of Chemistry and Biochemistry, University of California, San Diego
, La Jolla, California 92093, USA
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Raja Ghosh
;
Raja Ghosh
2
Department of Chemistry and Biochemistry, University of California, San Diego
, La Jolla, California 92093, USA
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Athanassios Z. Panagiotopoulos
;
Athanassios Z. Panagiotopoulos
a)
1
Department of Chemical and Biological Engineering, Princeton University
, Princeton, New Jersey 08544, USA
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Francesco Paesani
Francesco Paesani
b)
2
Department of Chemistry and Biochemistry, University of California, San Diego
, La Jolla, California 92093, USA
3
Materials Science and Engineering, University of California San Diego
, La Jolla, California 92093, USA
4
San Diego Supercomputer Center, University of California San Diego
, La Jolla, California 92093, USA
b)Author to whom correspondence should be addressed: [email protected]
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a)
Electronic mail: [email protected]
b)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 156, 104503 (2022)
Article history
Received:
November 28 2021
Accepted:
February 17 2022
Citation
Shuwen Yue, Marc Riera, Raja Ghosh, Athanassios Z. Panagiotopoulos, Francesco Paesani; Transferability of data-driven, many-body models for CO2 simulations in the vapor and liquid phases. J. Chem. Phys. 14 March 2022; 156 (10): 104503. https://doi.org/10.1063/5.0080061
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