Accelerating fourth-generation machine learning potentials by quasi-linear scaling particle mesh charge equilibration

Abstract: Machine learning potentials (MLP) have revolutionized the field of atomistic simulations by describing the atomic interactions with the accuracy of electronic structure methods at a small fraction of the costs. Most current MLPs construct the energy of a system as a sum of atomic energies, which depend on information about the atomic environments provided in form of predefined or learnable feature vectors. If, in addition, non-local phenomena like long-range charge transfer are important, fourth-generation MLPs need to be used, which include a charge equilibration (Qeq) step to take the global structure of the system into account. This Qeq can significantly increase the computational cost and thus can become the computational bottleneck for large systems. In this paper we present a highly efficient formulation of Qeq that does not require the explicit computation of the Coulomb matrix elements resulting in a quasi-linearly scaling method. Moreover, our approach also allows for the efficient calculation of energy derivatives, which explicitly consider the global structure-dependence of the atomic charges as obtained from Qeq. Due to its generality, the method is not restricted to MLPs but can also be applied within a variety of other force fields.