期刊
NATURE COMMUNICATIONS
卷 11, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-020-19093-1
关键词
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资金
- U.S. Army Research Office [W911NF-13-1-0387]
- Institute of Information & Communications Technology Planning & Evaluation (IITP) - Korea Government [2019-0-00079]
- Artificial Intelligence Graduate School Program, Korea University
- German Ministry for Education and Research (BMBF) [01IS14013A-E, 01GQ1115, 01GQ0850, 01IS18025A, 031L0207D, 01IS18037A]
- German Research Foundation (DFG) [EXC 2046/1, 390685689]
- NSF [CHE 1856165]
Kohn-Sham density functional theory (DFT) is a standard tool in most branches of chemistry, but accuracies for many molecules are limited to 2-3 kcal . mol(-1) with presently-available functionals. Ab initio methods, such as coupled-cluster, routinely produce much higher accuracy, but computational costs limit their application to small molecules. In this paper, we leverage machine learning to calculate coupled-cluster energies from DFT densities, reaching quantum chemical accuracy (errors below 1 kcal . mol(-1)) on test data. Moreover, density-based Delta -learning (learning only the correction to a standard DFT calculation, termed Delta -DFT ) significantly reduces the amount of training data required, particularly when molecular symmetries are included. The robustness of Delta -DFT is highlighted by correcting on the fly DFT-based molecular dynamics (MD) simulations of resorcinol (C6H4(OH)(2)) to obtain MD trajectories with coupled-cluster accuracy. We conclude, therefore, that Delta -DFT facilitates running gas-phase MD simulations with quantum chemical accuracy, even for strained geometries and conformer changes where standard DFT fails. High-level ab initio quantum chemical methods carry a high computational burden, thus limiting their applicability. Here, the authors employ machine learning to generate coupled-cluster energies and forces at chemical accuracy for geometry optimization and molecular dynamics from DFT densities.
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