COMPLAS 2023

GNN-Assisted Phase Space Integration with Application to Atomistics

  • Saxena, Shashank (ETH Zurich)
  • Bastek, Jan-Hendrik (ETH Zurich)
  • Spinola, Miguel (ETH Zurich)
  • Gupta, Prateek (IIT Delhi)
  • Kochmann, Dennis M (ETH Zurich)

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Overcoming the time scale limitations of atomistics can be achieved by switching from the state-space representation of Molecular Dynamics (MD) to a statistical-mechanics-based representation in phase space, where approximations such as maximum-entropy or Gaussian phase packets (GPP) evolve the atomistic ensemble in a time-coarsened fashion. In practice, this requires the computation of expensive high-dimensional integrals over all of phase space of an atomistic ensemble. This, in turn, is commonly accomplished efficiently by low-order numerical quadrature. We show that numerical quadrature in this context, unfortunately, comes with a set of inherent problems, which corrupt the accuracy of simulations---especially when dealing with crystal lattices with imperfections. As a remedy, we demonstrate that Graph Neural Networks, trained on Monte-Carlo data, can serve as a replacement for commonly used numerical quadrature rules, overcoming their deficiencies and significantly improving the accuracy. This is showcased by three benchmarks: the thermal expansion of copper, the martensitic phase transition of iron, and the energy of grain boundaries. We illustrate the benefits of the proposed technique over classically used third- and fifth-order Gaussian quadrature, we highlight the impact on time-coarsened atomistic predictions, and we discuss the computational efficiency. The latter is of general importance when performing frequent evaluations of phase space or other high-dimensional integrals, which is why the proposed framework promises applications beyond the scope of atomistics.