Simulation of large molecular systems with electronically-derived forces

Many-body electronic responses such as dispersion and polarization (at and beyond dipole order) present fundamental challenges in the simulation of materials at the molecular scale. To address these, an emerging strategy employing embedded quantum oscillators as a coarse-grained representation of such responses has been effective in predicting material properties with remarkable accuracy. However, applications have so far been limited to relatively small system sizes. Here we introduce strategies enabling efficient implementation of this framework on high-performance, heterogeneous CPU-GPU (with multiple Graphic Processing Units) computing platforms thereby increasing significantly the scale of accessible problems. Physical properties are reported for a benchmark system of 104 water molecules - to our knowledge, the largest system yet simulated using molecular dynamics with electronically-derived forces. (C) 2021 Elsevier B.V. All rights reserved.

Automated summary

A strategy using embedded quantum oscillators has been introduced to predict material properties with remarkable accuracy, efficiently implemented on high-performance computing platforms to significantly increase the scale of accessible problems. This approach has enabled simulations of the largest system yet using molecular dynamics with electronically-derived forces.