Tensorial Properties via the Neuroevolution Potential Framework: Fast Simulation of Infrared and Raman Spectra
Journal article, 2024
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.
Author
Nan Xu
College of Chemical and Biological Engineering, Zhejiang University
Institute of Zhejiang University-Quzhou
Petter Rosander
Chalmers, Physics, Condensed Matter and Materials Theory
Christian Schäfer
Chalmers, Physics, Condensed Matter and Materials Theory
Eric Lindgren
Chalmers, Physics, Condensed Matter and Materials Theory
Nicklas Österbacka
Chalmers, Physics, Condensed Matter and Materials Theory
Mandi Fang
College of Chemical and Biological Engineering, Zhejiang University
Institute of Zhejiang University-Quzhou
Wei Chen
Chinese Academy of Sciences
Yi He
UW College of Engineering
College of Chemical and Biological Engineering, Zhejiang University
Institute of Zhejiang University-Quzhou
Zheyong Fan
Bohai University
Paul Erhart
Chalmers, Physics, Condensed Matter and Materials Theory
Journal of Chemical Theory and Computation
1549-9618 (ISSN) 1549-9626 (eISSN)
Vol. 20 8 3273-3284Subject Categories
Theoretical Chemistry
DOI
10.1021/acs.jctc.3c01343
Related datasets
Data for "Tensorial properties via the neuroevolution potential framework: Fast simulation of infrared and Raman spectra" [dataset]
DOI: 10.5281/zenodo.10257363