Title: Machine learning of parameters for accurate semiempirical quantum chemical calculations

Abstract

We investigate possible improvements in the accuracy of semiempirical quantum chemistry (SQC) methods through the use of machine learning (ML) models for the parameters. For a given class of compounds, ML techniques require sufficiently large training sets to develop ML models that can be used for adapting SQC parameters to reflect changes in molecular composition and geometry. The ML-SQC approach allows the automatic tuning of SQC parameters for individual molecules, thereby improving the accuracy without deteriorating transferability to molecules with molecular descriptors very different from those in the training set. The performance of this approach is demonstrated for the semiempirical OM2 method using a set of 6095 constitutional isomers C₇H₁₀O₂, for which accurate ab initio atomization enthalpies are available. The ML-OM2 results show improved average accuracy and a much reduced error range compared with those of standard OM2 results, with mean absolute errors in atomization enthalpies dropping from 6.3 to 1.7 kcal/mol. They are also found to be superior to the results from specific OM2 reparameterizations (rOM2) for the same set of isomers. The ML-SQC approach thus holds promise for fast and reasonably accurate high-throughput screening of materials and molecules.

Authors:

Dral, Pavlo O. ^[1]; von Lilienfeld, O. Anatole ^[2]; Thiel, Walter ^[3]

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+ Show Author Affiliations

1. Max-Planck Institute fur Kohlenforschung, Mulheim an der Ruhr (Germany)
2. Univ. of Basel, Basel (Switzerland); Argonne National Lab. (ANL), Argonne, IL (United States)
3. Max-Planck Institute for Kohlenforschung, Mulheim an der Ruhr (Germany)

Publication Date:

Tue Apr 14 00:00:00 EDT 2015

Research Org.:

Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC)

OSTI Identifier:

1214088

Grant/Contract Number:  

AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

Journal of Chemical Theory and Computation

Additional Journal Information:

Journal Volume: 11; Journal Issue: 5; Journal ID: ISSN 1549-9618

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY