Fast and Robust Modeling of Lanthanide and Actinide Complexes, Biomolecules, and Molecular Crystals with the Extended GFN-FF Model

Abstract

Lanthanides (Ln) and actinides (An) have recently become important tools in biomedical and materials science. However, the development of computational methods able to describe such elements in various environments has not kept up with the pace of the field. Addressing this challenge, this work introduces and showcases an extension of the GFN-FF to An alongside a reparameterization for Ln. This development fills a gap for fast computational methods that are out-of-the-box applicable to large f-element-containing systems with thousands of atoms. We discuss the reparameterization of the charge model and the covalent topology setup and showcase the model through various applications: Molecular dynamics simulations, optimization of Ln-containing biomolecules, and optimizations of several periodic structures. With the presented improvements, GFN-FF is a powerful method that routinely delivers robust and accurate geometries for large Ln/An systems with thousands of atoms.