A universal density matrix functional from molecular orbital-based machine learning: Transferability across organic molecules
Abstract
We address the degree to which machine learning (ML) can be used to accurately and transferably predict post-Hartree-Fock correlation energies. Refined strategies for feature design and selection are presented, and the molecular-orbital-based machine learning (MOB-ML) method is applied to several test systems. Strikingly, for the second-order Møller-Plessett perturbation theory, coupled cluster with singles and doubles (CCSD), and CCSD with perturbative triples levels of theory, it is shown that the thermally accessible (350 K) potential energy surface for a single water molecule can be described to within 1 mhartree using a model that is trained from only a single reference calculation at a randomized geometry. To explore the breadth of chemical diversity that can be described, MOB-ML is also applied to a new dataset of thermalized (350 K) geometries of 7211 organic models with up to seven heavy atoms. In comparison with the previously reported Δ-ML method, MOB-ML is shown to reach chemical accuracy with threefold fewer training geometries. Finally, a transferability test in which models trained for seven-heavy-atom systems are used to predict energies for thirteen-heavy-atom systems reveals that MOB-ML reaches chemical accuracy with 36-fold fewer training calculations than Δ-ML (140 vs 5000 training calculations).
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Apr 04, 2019
- Source ID
- 10.1063/1.5088393
Entities
People
- Anders S Christensen
- Lixue Cheng
- Matthew Welborn
- Thomas Miller
Organizations
- Air Force Office of Scientific Research
- California Institute of Technology
- Institute of Physical Chemistry, Polish Academy of Sciences
- Swiss National Science Foundation
- United States Department of Energy