Molecular simulation by knowledgeable quantum atoms

TLDR: The next-next-generation force field (QCTFF) as mentioned in this paper is a force field based on the atomistic kriging model, which can learn how fundamental energy quantities, as well as high-rank multipole moments, all associated with an atom of interest, vary with the precise positions of atomic neighbors.

Abstract: We are at the dawn of molecular simulations being carried out, literally, by atoms endowed by knowledge of how to behave quantum mechanically in the vicinity of other atoms. The 'next–next-generation' force field that aims to achieve this is called QCTFF, for now, although a more pronounceable name will be suggested in the conclusion. Classical force fields such as AMBER mimic the interatomic energy experienced by atoms during a molecular simulation, with simple expressions capturing a relationship between energy and nuclear position. Such force fields neither see the electron density nor exchange-delocalization itself, or exact electrostatic interaction; they only contain simple equations and elementary parameters such as point charges to imitate the energies between atoms. Next-generation force fields, such as AMOEBA, go further and make the electrostatics more accurate by introducing multipole moments and dipolar polarization. However, QCTFF goes even further and abolishes all traditional force field expressions (e.g. Hooke's law and extensions, Lennard-Jones) in favor of atomistic kriging models. These machine learning models learn how fundamental energy quantities, as well as high-rank multipole moments, all associated with an atom of interest, vary with the precise positions of atomic neighbors. As a result, all structural phenomena can be rapidly calculated as an interplay of intra-atomic energy, exchange-delocalization energy, electrostatic energy and dynamic correlation energy. The final QCTFF force field will generate a wealth of localized quantum information while being faster than a Car–Parrinello simulation (which does not generate local information). Isn't it enough to see that a garden is beautiful without having to believe that there are fairies at the bottom of it too? (Douglas Adams).