Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 156, Issue 16, Pages -Publisher
AIP Publishing
DOI: 10.1063/5.0090862
Keywords
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Science [DE-SC0019490]
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- Extreme Science and Engineering Discovery Environment (XSEDE)
- National Science Foundation [ACI-1548562]
- Triton Shared Computing Cluster (TSCC) at the San Diego Supercomputer Center (SDSC)
- Alfred P. Sloan Foundation Graduate Fellowship Program
- U.S. Department of Energy (DOE) [DE-SC0019490] Funding Source: U.S. Department of Energy (DOE)
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Recent research has shown that the deep-learned DM21 functional can overcome the delocalization error of traditional DFAs, but its ability to accurately predict the energetics of water clusters varies significantly with cluster size. Additionally, the size-dependent functional-driven errors identified in the analysis of small clusters calculated with the DM21 functional result in the MB-DM21 potential systematically overestimating the hydrogen-bond strength when used in simulations of liquid water.
The delicate interplay between functional-driven and density-driven errors in density functional theory (DFT) has hindered traditional density functional approximations (DFAs) from providing an accurate description of water for over 30 years. Recently, the deep-learned DeepMind 21 (DM21) functional has been shown to overcome the limitations of traditional DFAs as it is free of delocalization error. To determine if DM21 can enable a molecular-level description of the physical properties of aqueous systems within Kohn-Sham DFT, we assess the accuracy of the DM21 functional for neutral, protonated, and deprotonated water clusters. We find that the ability of DM21 to accurately predict the energetics of aqueous clusters varies significantly with cluster size. Additionally, we introduce the many-body MB-DM21 potential derived from DM21 data within the many-body expansion of the energy and use it in simulations of liquid water as a function of temperature at ambient pressure. We find that size-dependent functional-driven errors identified in the analysis of the energetics of small clusters calculated with the DM21 functional result in the MB-DM21 potential systematically overestimating the hydrogen-bond strength and, consequently, predicting a more ice-like local structure of water at room temperature. Published under an exclusive license by AIP Publishing
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