Quantum chemical benchmark databases of gold-standard dimer interaction energies

Alexander G Donchev,John L Klepeis,Andrew G Taube,Ka-Hei Law,Elizabeth Decolvenaere,Karthik Siva,Cory Hargus,David E Shaw,Je-Luen Li,Michael Bergdorf,Robert T Mcgibbon,Kim Palmo,Brent A Gregersen

doi:10.1038/s41597-021-00833-x

Alexander G Donchev, John L Klepeis + Show 11 more

Open Access

https://doi.org/10.1038/s41597-021-00833-x

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Journal: Scientific Data	Publication Date: Feb 10, 2021
Citations: 36	License type: open-access

Affiliation: D. E. Shaw Research, Columbia University

Abstract

Advances in computational chemistry create an ongoing need for larger and higher-quality datasets that characterize noncovalent molecular interactions. We present three benchmark collections of quantum mechanical data, covering approximately 3,700 distinct types of interacting molecule pairs. The first collection, which we refer to as DES370K, contains interaction energies for more than 370,000 dimer geometries. These were computed using the coupled-cluster method with single, double, and perturbative triple excitations [CCSD(T)], which is widely regarded as the gold-standard method in electronic structure theory. Our second benchmark collection, a core representative subset of DES370K called DES15K, is intended for more computationally demanding applications of the data. Finally, DES5M, our third collection, comprises interaction energies for nearly 5,000,000 dimer geometries; these were calculated using SNS-MP2, a machine learning approach that provides results with accuracy comparable to that of our coupled-cluster training data. These datasets may prove useful in the development of density functionals, empirically corrected wavefunction-based approaches, semi-empirical methods, force fields, and models trained using machine learning methods.

Highlights

Experimental means of quantifying individual noncovalent interactions are limited to small systems with relatively rigid intramolecular degrees of freedom[1], and computer simulations offer a much-needed alternative; quantum mechanical (QM) calculations, for example, enable the characterization of noncovalent interactions with high accuracy
Among QM-based approaches, the use of coupled-cluster singles and doubles with perturbative triples [CCSD(T)]2–4 at the complete basis set (CBS) limit is widely recognized as the gold-standard method for noncovalent interactions[4]
The DES5M collection contains 4,955,938 additional unique geometries originating from the same two sources as were used for DES370K: radial profiles starting from a set of QM-optimized conformers and dimer geometries extracted from molecular dynamics (MD) simulations

Summary

Introduction

Because many potential applications of the presented data, such as parameterizing a new exchange-correlation functional, are computationally demanding, we compiled DES15K, a core subset of the most representative structures from DES370K that largely retains the chemical and orientational diversity of DES370K, but with reduced resolution of scan points in the radial profiles (Table 1). We found[39] that for dimer interaction energies, the SNS-MP2 method offers—at a greatly reduced cost—accuracy comparable to that of the CCSD(T)/CBS approach used to obtain the benchmark data in DES370K.

Results

Conclusion