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Tensorial properties via the neuroevolution potential framework: Fast simulation of infrared and Raman spectra

Published 8 Dec 2023 in cond-mat.mes-hall, cond-mat.mtrl-sci, physics.chem-ph, and physics.comp-ph | (2312.05233v2)

Abstract: 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 application range and reliability. Here, we introduce a ML accelerated approach that addresses these shortcomings and provides a significant performance boost in terms of data and computational efficiency compared to 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.

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References (44)
  1. B. Schrader, Infrared and Raman spectroscopy: Methods and applications, Vibrational Spectroscopy of Different Classes and States of Compounds (Wiley-VCH, 1995).
  2. R. S. Das and Y. Agrawal, Vib. Spectrosc. 57, 163 (2011).
  3. P. L. Silvestrelli, M. Bernasconi, and M. Parrinello, Chem. Phys. Lett. 277, 478 (1997).
  4. A. Putrino and M. Parrinello, Phys. Rev. Lett. 88, 176401 (2002).
  5. S. Luber, M. Iannuzzi, and J. Hutter, J. Chem. Phys. 141, 094503 (2014).
  6. A. D. MacKerell Jr., N. Banavali, and N. Foloppe, Biopolymers 56, 257 (2000).
  7. W. L. Jorgensen and J. Tirado-Rives, J. Am. Chem. Soc. 110, 1657 (1988).
  8. S. M. Foiles, M. I. Baskes, and M. S. Daw, Phys. Rev. B 33, 7983 (1986).
  9. J. Tersoff, Phys. Rev. Lett. 61, 2879 (1988).
  10. J. Behler, J. Chem. Phys. 145, 170901 (2016).
  11. Y. Zhang, J. Xia, and B. Jiang, Phys. Rev. Lett. 127, 156002 (2021a).
  12. M. Gastegger, J. Behler, and P. Marquetand, Chem. Sci. 8, 6924 (2017).
  13. K. Kwac, H. Freedman, and M. Cho, J. Chem. Theory Comput. 17, 6353 (2021).
  14. I. Leontyev and A. Stuchebrukhov, Phys. Chem. Chem. Phys. 13, 2613 (2011).
  15. K. S. Smirnov and D. Bougeard, J. Raman Spectrosc. 37, 100 (2006).
  16. Q. Chen and S. T. Milner, Macromolecules 50, 9773 (2017).
  17. P. Bornhauser and D. Bougeard, J. Raman Spectrosc. 32, 279 (2001).
  18. D. Bougeard and K. S. Smirnov, J. Raman Spectrosc. 40, 1704 (2009).
  19. T. Hasegawa and Y. Tanimura, J. Phys. Chem. B 115, 5545 (2011).
  20. G. R. Medders and F. Paesani, J. Chem. Theory Comput. 11, 1145 (2015).
  21. E. Berger, Z.-P. Lv, and H.-P. Komsa, J. Mater. Chem. C 11, 1311 (2023).
  22. E. Berger and H.-P. Komsa, Polarizability Models for Simulations of Finite Temperature Raman Spectra from Machine Learning Molecular Dynamics (2023), arxiv:2310.13310 [cond-mat, physics:physics] .
  23. Z. Fan, J. Phys. Condens. Matter 34, 125902 (2022).
  24. J. Behler and M. Parrinello, Phys. Rev. Lett. 98, 146401 (2007).
  25. D. A. McQuarrie, Statistical Mechanics, Harper’s chemistry series (Harper Collins, New York, 1976).
  26. TENSOAP (accessed: 12-08-2023a), https://github.com/dilkins/TENSOAP.
  27. TENSOAP-FAST (accessed: 12-08-2023b), https://github.com/dilkins/TENSOAP-FAST/tree/master/example/models/bulk-water.
  28. G. Makov and M. C. Payne, Phys. Rev. B 51, 4014 (1995).
  29. E. Ditler, J. Mattiat, and S. Luber, Phys. Chem. Chem. Phys. 25, 14672 (2023).
  30. in Ideas of Quantum Chemistry, edited by L. Piela (Elsevier, Amsterdam, 2007) pp. 615–680.
  31. N. A. Spaldin, J. Solid State Chem. 195, 2 (2012).
  32. NEP_CPU (accessed: 12-08-2023), https://github.com/brucefan1983/NEP_CPU.
  33. calorine (accessed: 12-08-2023), https://calorine.materialsmodeling.org/; DOI: 10.5281/zenodo.7919206.
  34. M. Praprotnik and D. Janežič, J. Chem. Phys. 122, 174103 (2005).
  35. H. D. Downing and D. Williams, J. Geophys. Res. 80, 1656 (1975).
  36. J.-J. Max and C. Chapados, J. Chem. Phys. 131, 184505 (2009).
  37. A. Rognoni, R. Conte, and M. Ceotto, Chem. Sci. 12, 2060 (2021).
  38. M. Praprotnik, D. Janežič, and J. Mavri, J. Phys. Chem. A 108, 11056 (2004).
  39. J. Sun, A. Ruzsinszky, and J. P. Perdew, Phys. Rev. Lett. 115, 036402 (2015).
  40. V. R. Chintareddy, K. Wadhwa, and J. G. Verkade, J. Org. Chem 76, 4482 (2011).
  41. J. P. Perdew, K. Burke, and M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996).
  42. F. Weigend and A. Baldes, J. Chem. Phys. 133 (2010).
  43. K. S. Knight, Journal of Materials Science 55, 6417 (2020).
  44. K. Berland and P. Hyldgaard, Physical Review B 89, 035412 (2014).
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