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Title: Constructing High-Dimensional Neural Network Potential Energy Surfaces for Gas–Surface Scattering and Reactions

Journal Article · · Journal of Physical Chemistry. C

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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE; National Science Foundation (NSF)
OSTI ID:
1483684
Journal Information:
Journal of Physical Chemistry. C, Vol. 122, Issue 3; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 71 works
Citation information provided by
Web of Science

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Vibrational enhancement in the dynamics of ammonia dissociative chemisorption on Ru(0001) journal July 2018
Hot-electron effects during reactive scattering of H 2 from Ag(111): the interplay between mode-specific electronic friction and the potential energy landscape journal January 2019
Dissociation of CHD 3 on Cu(111), Cu(211), and single atom alloys of Cu(111) journal December 2018
A modified generalized Langevin oscillator model for activated gas-surface reactions journal January 2019
Dynamics in reactions on metal surfaces: A theoretical perspective journal May 2019
Iterative training set refinement enables reactive molecular dynamics via machine learned forces journal January 2020
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A facile strategy to realize a single/double photon excitation-dependent photosensitizer for imaging-guided phototherapy against HeLa cancer cells at separate irradiation channels journal January 2020
Correlation of structure with UV-visible spectra by varying SH composition in Au-SH nanoclusters journal August 2018
Continuous and optimally complete description of chemical environments using Spherical Bessel descriptors journal January 2020
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Figures / Tables (7)