Developing a User-Friendly Code for the Fast Estimation of Well-Behaved Real-Space Partial Charges

Abstract

The Quantum Theory of Atoms in Molecules (QTAIM) provides an intuitive, yet physically sound, strategy to determine the partial charges of any chemical system relying on the topology induced by the electron density ρ(r) . In a previous work [J. Chem. Phys. 2022, 156, 014112], we introduced a machine learning (ML) model for the computation of QTAIM charges of C, H, O, and N atoms at a fraction of the conventional computational cost. Unfortunately, the independent nature of the atomistic predictions implies that the raw atomic charges may not necessarily reconstruct the exact molecular charge, limiting the applicability of the latter in the chemistry realm. Trying to solve such an inconvenience, we introduce NNAIMGUI, a user-friendly code which combines the inferring abilities of ML with an equilibration strategy to afford adequately behaved partial charges. The performance of this approach is put to the test in a variety of scenarios including interpolation and extrapolation regimes (e.g chemical reactions) as well as large systems. The results of this work prove that the equilibrated charges retain the chemically accurate behavior reproduced by the ML models. Furthermore, NNAIMGUI is a fully flexible architecture allowing users to train and use tailor-made models targeted at any atomic property of choice. In this way, the GUI-interfaced code, equipped with visualization utilities, makes the computation of real-space atomic properties much more appealing and intuitive, paving the way toward the extension of QTAIM related descriptors beyond the theoretical chemistry community.