Designing Accurate Moment Tensor Potentials for Phonon-Related Properties of Crystalline Polymers.

ABSTRACT

The phonon-related properties of crystalline polymers are highly relevant for various applications. Their simulation is, however, particularly challenging, as the systems that need to be modeled are often too extended to be treated by ab initio methods, while classical force fields are too inaccurate. Machine-learned potentials parametrized against material-specific ab initio data hold the promise of being extremely accurate and also highly efficient. Still, for their successful application, protocols for their parametrization need to be established to ensure an optimal performance, and the resulting potentials need to be thoroughly benchmarked. These tasks are tackled in the current manuscript, where we devise a protocol for parametrizing moment tensor potentials (MTPs) to describe the structural properties, phonon band structures, elastic constants, and forces in molecular dynamics simulations for three prototypical crystalline polymers polyethylene (PE), polythiophene (PT), and poly-3-hexylthiophene (P3HT). For PE, the thermal conductivity and thermal expansion are also simulated and compared to experiments. A central element of the approach is to choose training data in view of the considered use case of the MTPs. This not only yields a massive speedup for complex calculations while essentially maintaining DFT accuracy, but also enables the reliable simulation of properties that, so far, have been entirely out of reach.