While the ab initio molecular dynamics (AIMD) approach to gas–surface interaction has been instrumental in exploring important issues such as energy transfer and reactivity, it is only amenable to short-time events and a limited number of trajectories because of the on-the-fly nature of the density functional theory (DFT) calculations. In this work, we report a high-dimensional global reactive potential energy surface (PES) constructed with high fidelity from judiciously placed DFT points, using a machine learning method; and it is orders-of-magnitude more efficient than AIMD in dynamical calculations and can be employed in various simulations without performing additional electronic structure calculations. Importantly, the surface atoms are included in such a PES, which provides a unique platform for studying energy transfer and scattering/reaction of the impinging molecule on the solid surface on an equal footing.
Liu, Qinghua, Zhou, Xueyao, Zhou, Linsen, et al., "Constructing High-Dimensional Neural Network Potential Energy Surfaces for Gas–Surface Scattering and Reactions," Journal of Physical Chemistry. C 122, no. 3 (2018), https://doi.org/10.1021/acs.jpcc.7b12064
@article{osti_1483684,
author = {Liu, Qinghua and Zhou, Xueyao and Zhou, Linsen and Zhang, Yaolong and Luo, Xuan and Guo, Hua and Jiang, Bin},
title = {Constructing High-Dimensional Neural Network Potential Energy Surfaces for Gas–Surface Scattering and Reactions},
annote = {While the ab initio molecular dynamics (AIMD) approach to gas–surface interaction has been instrumental in exploring important issues such as energy transfer and reactivity, it is only amenable to short-time events and a limited number of trajectories because of the on-the-fly nature of the density functional theory (DFT) calculations. In this work, we report a high-dimensional global reactive potential energy surface (PES) constructed with high fidelity from judiciously placed DFT points, using a machine learning method; and it is orders-of-magnitude more efficient than AIMD in dynamical calculations and can be employed in various simulations without performing additional electronic structure calculations. Importantly, the surface atoms are included in such a PES, which provides a unique platform for studying energy transfer and scattering/reaction of the impinging molecule on the solid surface on an equal footing.},
doi = {10.1021/acs.jpcc.7b12064},
url = {https://www.osti.gov/biblio/1483684},
journal = {Journal of Physical Chemistry. C},
issn = {ISSN 1932-7447},
number = {3},
volume = {122},
place = {United States},
publisher = {American Chemical Society},
year = {2018},
month = {01}}
