Tensorial Properties via the Neuroevolution Potential Framework: Fast Simulation of Infrared and Raman Spectra
Artikel i vetenskaplig tidskrift, 2023
Infrared and Raman spectroscopy are widely used for the characterization of gases, liquids, and solids, as the spectra contain a wealth of information concerning, in particular, the dynamics of these systems. Atomic scale simulations can be used to predict such spectra but are often severely limited due to high computational cost or the need for strong approximations that limit the application range and reliability. Here, we introduce a machine learning (ML) accelerated approach that addresses these shortcomings and provides a significant performance boost in terms of data and computational efficiency compared with earlier ML schemes. To this end, we generalize the neuroevolution potential approach to enable the prediction of rank one and two tensors to obtain the tensorial neuroevolution potential (TNEP) scheme. We apply the resulting framework to construct models for the dipole moment, polarizability, and susceptibility of molecules, liquids, and solids and show that our approach compares favorably with several ML models from the literature with respect to accuracy and computational efficiency. Finally, we demonstrate the application of the TNEP approach to the prediction of infrared and Raman spectra of liquid water, a molecule (PTAF-), and a prototypical perovskite with strong anharmonicity (BaZrO3). The TNEP approach is implemented in the free and open source software package gpumd, which makes this methodology readily available to the scientific community.
Författare
Nan Xu
Institute of Zhejiang University-Quzhou
College of Chemical and Biological Engineering, Zhejiang University
Petter Rosander
Chalmers, Fysik, Kondenserad materie- och materialteori
Christian Schäfer
Chalmers, Fysik, Kondenserad materie- och materialteori
Eric Lindgren
Chalmers, Fysik, Kondenserad materie- och materialteori
Nicklas Österbacka
Chalmers, Fysik, Kondenserad materie- och materialteori
Mandi Fang
Institute of Zhejiang University-Quzhou
College of Chemical and Biological Engineering, Zhejiang University
Wei Chen
Institute of Process Engineering Chinese Academy of Sciences
Yi He
College of Chemical and Biological Engineering, Zhejiang University
Institute of Zhejiang University-Quzhou
UW College of Engineering
Zheyong Fan
Bohai University
Paul Erhart
Chalmers, Fysik, Kondenserad materie- och materialteori
Journal of Chemical Theory and Computation
1549-9618 (ISSN) 1549-9626 (eISSN)
Vol. In PressÄmneskategorier
Teoretisk kemi
DOI
10.1021/acs.jctc.3c01343