期刊
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
卷 16, 期 12, 页码 7462-7472出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.0c00932
关键词
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资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Science [DE-SC0019490]
- National Science Foundation [1704063]
- NIGMS/NIH [R01GM108583]
- Gaussian, Inc.
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- Triton Shared Computing Cluster (TSCC) at the San Diego Supercomputer Center (SDSC)
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1704063] Funding Source: National Science Foundation
We present a new development in quantum mechanics/molecular mechanics (QM/MM) methods by replacing conventional MM models with data-driven many-body (MB) representations rigorously derived from high-level QM calculations. The new QM/MM approach builds on top of mutually polarizable QM/ MM schemes developed for polarizable force fields with inducible dipoles and uses permutationally invariant polynomials to effectively account for quantum-mechanical contributions (e.g., exchange-repulsion and charge transfer and penetration) that are difficult to describe by classical expressions adopted by conventional MM models. Using the many-body MB-pol and MB-DFT potential energy functions for water, which include explicit two-body and three-body terms fitted to reproduce the corresponding CCSD(T) and PBEO two-body and three-body energies for water, we demonstrate a smooth energetic transition as molecules are transferred between QM and MM regions, without the need of a transition layer. By effectively elevating the accuracy of both the MM region and the QM/MM interface to that of the QM region, the new QM/MB-MM approach achieves an accuracy comparable to that obtained with a fully QM treatment of the entire system.
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