VibML

The deposited data sets were used to obtain representations
of potential energy surfaces (PESs) for eight representative
molecules using a neural network of the PhysNet type [1]. The
molecules under investigation are H2CO, trans-HONO, HCOOH,
CH3OH, CH3CHO, CH3NO2, CH3COOH and CH3CONH2.

Reference data calculated at three different levels of quantum
chemical theory (MP2/aug-cc-pVTZ, CCSD(T)/aug-cc-pVTZ and
CCSD(T)-F12/aug-cc-pVTZ-F12) was used to train machine learning
(ML) models. Data sets at the MP2 level of theory were generated
for all molecules, at CCSD(T) level they were generated for
molecules with less than 7 atoms, and data sets at the CCSD(T)-F12
level of theory were generated for molecules with less than 6
atoms. The data sets contain different geometries for each
molecule generated using the normal mode sampling approach [2]
performed at different temperatures. The ab initio calculations
were performed using MOLPRO [3].

The performance of the PhysNet is then examined by considering
out-of-sample energy and force errors, harmonic frequencies in
comparison to explicit ab initio calculations and anharmonic
frequencies (obtained from a second order vibrational perturbation
theory (VPT2) analysis [4] as implemented in the Gaussian 09
suite [5]) in comparison to ab initio VPT2 calculations at the
MP2 level as well as to experiment.

For more details, see https://arxiv.org/abs/2103.05491

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HOW TO CITE:

When using this dataset, please cite the following paper:
Käser, S. and Boittier, E. and Upadhyay, M. and Meuwly, M.
"MP2 Is Not Good Enough! Transfer Learning ML Models for
Accurate VPT2 Frequencies", arXiv:2103.05491.

and the digital object identifier (DOI):
Käser, S. and Boittier, E. and Upadhyay, M. and Meuwly, M. (2021).
VibML. Zenodo. http://doi.org/10.5281/zenodo.4585449

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[1] Unke, O. T.; Meuwly, M. J. Chem. Theory Comput. 2019, 15, 3678–3693
[2] Smith, J. S.; Isayev, O.; Roitberg, A. E. Sci. Data 2017, 4, 170193
[3] Werner, H.-J.; Knowles, P. J.; Knizia, G.; Manby, F. R.; Schütz, M.; et al. https://www.molpro.net
[4] Barone, V.; J. Chem. Phys. 2005, 122, 014108
[5] Frisch, M. J.;  Trucks, G. W.;  Schlegel, H. B.;  Scuseria, G. E.;  Robb, M. A.;  Cheeseman, J. R.;
    Scalmani, G.; Barone, V.; Mennucci, B.; Petersson, G. A. et al. Gaussian09 Revision E.01. Gaussian Inc.
    Wallingford CT 2009