O(N) Stochastic Evaluation of Many-Body van der Waals Energies in Large Complex Systems
Pier Paolo Poier, Louis Lagardère, Jean‐Philip Piquemal
Abstract
We propose a new strategy to solve the key equations of the many-body dispersion (MBD) model by Tkatchenko, DiStasio Jr., and Ambrosetti. Our approach overcomes the original O(N3) computational complexity that limits its applicability to large molecular systems within the context of O(N) density functional theory. First, to generate the required frequency-dependent screened polarizabilities, we introduce an efficient solution to the Dyson-like self-consistent screening equations. The scheme reduces the number of variables and, coupled to a direct inversion of the iterative subspace extrapolation, exhibits linear-scaling performances. Second, we apply a stochastic Lanczos trace estimator resolution to the equations evaluating the many-body interaction energy of coupled quantum harmonic oscillators. While scaling linearly, it also enables communication-free pleasingly parallel implementations. As the resulting O(N) stochastic massively parallel MBD approach is found to exhibit minimal memory requirements, it opens up the possibility of computing accurate many-body van der Waals interactions of millions-atoms’ complex materials and solvated biosystems with computational times in the range of minutes.