A fast neural network approach for direct covariant forces prediction in complex multi-element extended systems

Abstract

Neural network force field (NNFF) is a method for performing regression on atomic structure–force relationships, bypassing the expensive quantum mechanics calculations that prevent the execution of long ab initio quality molecular dynamics (MD) simulations. However, most NNFF methods for complex multi-element atomic systems indirectly predict atomic force vectors by exploiting just atomic structure rotation-invariant features and network-feature spatial derivatives, which are computationally expensive. Here, we show a staggered NNFF architecture that exploits both rotation-invariant and -covariant features to directly predict atomic force vectors without using spatial derivatives, and we demonstrate 2.2× NNFF–MD acceleration over a state-of-the-art C++ engine using a Python engine. This fast architecture enables us to develop NNFF for complex ternary- and quaternary-element extended systems composed of long polymer chains, amorphous oxide and surface chemical reactions. The rotation-invariant–covariant architecture described here can also directly predict complex covariant vector outputs from local environments, in other domains beyond computational material science.

A preprint version of the article is available at ArXiv.

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Fig. 1: Comparison of the DCF algorithm and a standard B–P NNFF approach.
Fig. 2: DCF training algorithm.
Fig. 3: Demonstrated DCF material systems and regression performance.
Fig. 4: Demonstrated DCF MD speed and dynamics validation.
Fig. 5: DCF regression performance on chemical reaction snapshots.

Data availability

The atomic structure–force dataset (for systems A, B and C) is available through a Code Ocean compute capsule (https://doi.org/10.24433/CO.2788051.v1). The Python code for training the NNFF of the DCF approach of this work is available through a Code Ocean compute capsule (https://doi.org/10.24422/CO.2788051.v1).

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Acknowledgements

We thank S. Falkner and C. Cunha from the Bosch Center for Artificial Intelligence (BCAI) for feedback on NNFF algorithm accuracy improvement. This research used resources of the Oak Ridge Leadership Computing Facility at Oak Ridge National Laboratory, which is supported by the Office of Science of the Department of Energy under contract DE-AC05-00OR22725. The research was partially funded by the Advanced Research Projects Agency – Energy (ARPA-E), US Department of Energy, under award no. DE-AR0000775.

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J.P.M. conceived and implemented the staggered rotation-invariant and -covariant feature separation algorithm. J.P.M., M.K., G.S., S.T.L., C.A. and N.M. generated the training and test datasets for systems A, B and C. J.P.M. evaluated the NNFF accuracy. S.L.B., J.P.M. and M.K. performed the computational cost analysis. S.T.L. developed the HMM for generation of the system C reaction dataset. J.P.M., S.L.B. and J.V. built the DCF Python-based MD engine. M.K. developed the DCF Fortran acceleration for Python. J.P.M. performed the DCF MD study and error analysis. B.K. mentors the research at Bosch and is the primary academic supervisor for S.L.B. and J.V. on this work. J.P.M. wrote the manuscript. All authors contributed to manuscript preparation.

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Correspondence to Jonathan P. Mailoa or Boris Kozinsky.

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Mailoa, J.P., Kornbluth, M., Batzner, S. et al. A fast neural network approach for direct covariant forces prediction in complex multi-element extended systems. Nat Mach Intell 1, 471–479 (2019). https://doi.org/10.1038/s42256-019-0098-0

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