We use the MB-pol theoretical/computational framework to introduce a new family of data-driven many-body potential energy functions (PEFs) for water, named MB-pol(2023). By employing larger 2-body and 3-body training sets, including an explicit machine-learned representation of 4-body energies, and adopting more sophisticated machine-learned representations of 2-body and 3-body energies, we demonstrate that the MB-pol(2023) PEFs achieve sub-chemical accuracy in modeling the energetics of the hexamer isomers, outperforming both the original MB-pol and q-AQUA PEFs, which currently provide the most accurate description of water clusters in the gas phase. Importantly, the MB-pol(2023) PEFs provide remarkable agreement with the experimental results for various properties of liquid water, improving upon the original MB-pol PEF and effectively closing the gap with experimental measurements.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1021/acs.jctc.3c00326 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Prospects for rank-reduced CCSD(T) in the context of high-accuracy thermochemistry.
J Chem Phys
October 2024
Department of Chemistry, Southern Methodist University, Dallas, Texas 75275, USA.
Obtaining sub-chemical accuracy (1 kJ mol-1) for reaction energies of medium-sized gas-phase molecules is a longstanding challenge in the field of thermochemical modeling. The perturbative triples correction to coupled-cluster single double triple [CCSD(T)] constitutes an important component of all high-accuracy composite model chemistries that obtain this accuracy but can be a roadblock in the calculation of medium to large systems due to its O(N7) scaling, particularly in HEAT-like model chemistries that eschew separation of core and valence correlation. This study extends the work of Lesiuk [J.
View Article and Find Full Text PDFMB-pol(2023): Sub-chemical Accuracy for Water Simulations from the Gas to the Liquid Phase.
J Chem Theory Comput
June 2023
Department of Chemistry and Biochemistry, University of California San Diego, La Jolla, California 92093, United States.
We use the MB-pol theoretical/computational framework to introduce a new family of data-driven many-body potential energy functions (PEFs) for water, named MB-pol(2023). By employing larger 2-body and 3-body training sets, including an explicit machine-learned representation of 4-body energies, and adopting more sophisticated machine-learned representations of 2-body and 3-body energies, we demonstrate that the MB-pol(2023) PEFs achieve sub-chemical accuracy in modeling the energetics of the hexamer isomers, outperforming both the original MB-pol and q-AQUA PEFs, which currently provide the most accurate description of water clusters in the gas phase. Importantly, the MB-pol(2023) PEFs provide remarkable agreement with the experimental results for various properties of liquid water, improving upon the original MB-pol PEF and effectively closing the gap with experimental measurements.
View Article and Find Full Text PDFDevelopment of accurate potentials for the physisorption of water on graphene.
J Chem Phys
January 2023
Departamento de Química Física, Universidad de Valencia, Avda. Dr. Moliner 50, E-46100 Burjassot, Spain.
From coupled-cluster singles and doubles model including connected triples corrections [CCSD(T)] calculations on the water dimer and B97D/CC on the water-circumcoronene complex at a large number of randomly generated conformations, interaction potentials for the physisorption of water on graphene are built, accomplishing almost sub-chemical accuracy. The force fields were constructed by decomposing the interaction into electrostatic and van der Waals contributions, the latter represented through improved Lennard-Jones potentials. Besides, a Chemistry at Harvard Macromolecular Mechanics (CHARMM)-like term was included in the water-water potential to improve the description of hydrogen bonds, and an induction term was added to model the polarization effects in the interaction between water and polyaromatic hydrocarbons (PAHs) or graphene.
View Article and Find Full Text PDFDMC-ICE13: Ambient and high pressure polymorphs of ice from diffusion Monte Carlo and density functional theory.
J Chem Phys
October 2022
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, United Kingdom.
Ice is one of the most important and interesting molecular crystals, exhibiting a rich and evolving phase diagram. Recent discoveries mean that there are now 20 distinct polymorphs; a structural diversity that arises from a delicate interplay of hydrogen bonding and van der Waals dispersion forces. This wealth of structures provides a stern test of electronic structure theories, with Density Functional Theory (DFT) often not able to accurately characterize the relative energies of the various ice polymorphs.
View Article and Find Full Text PDFS2 Reactions with an Ambident Nucleophile: A Benchmark Ab Initio Study of the CN + CHY [Y = F, Cl, Br, and I] Systems.
J Phys Chem A
February 2022
MTA-SZTE Lendület Computational Reaction Dynamics Research Group, Interdisciplinary Excellence Centre and Department of Physical Chemistry and Materials Science, Institute of Chemistry, University of Szeged, Rerrich Béla tér 1, Szeged H-6720, Hungary.
We characterize the Walden-inversion, front-side attack, and double-inversion S2 pathways leading to Y + CHCN/CHNC and the product channels of proton abstraction (HCN/HNC + CHY), hydride-ion substitution (H + YHCCN/YHCNC), halogen abstraction (YCN/YNC + CH and YCN/YNC + CH), and YHCN/YHNC complex formation (YHCN/YHNC + CH) of the CN + CHY [Y = F, Cl, Br, and I] reactions. Benchmark structures and frequencies are computed at the CCSD(T)-F12b/aug-cc-pVTZ level of theory, and a composite approach is employed to obtain relative energies with sub-chemical accuracy considering (a) basis-set effects up to aug-cc-pVQZ, (b) post-CCSD(T) correlation up to CCSDT(Q), (c) core correlation, (d) relativistic effects, and (e) zero-point energy corrections. C-C bond formation is both thermodynamically and kinetically more preferred than N-C bond formation, though the kinetic preference is less significant.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!