Preprint

Effective Atom Theory: gradient-driven ab initio materials design

Tahmassebpur, J., Li, B., Barron, B., Abruña, H., Frazier, P., Arias, T.

arXiv e-prints 2509.07180
6 pages.
arXiv
submitted on: 08 September 2025 (version 1) (2025), unpublished

DOI:10.48550/arXiv.2509.07180

Open Access

Abstract

We introduce Effective Atom Theory (EAT), a framework that transforms combinatorial materials design into a smooth, gradient-driven optimization within density-functional theory (DFT). Atoms are represented as probabilistic mixtures of species/elements, enabling gradient-based optimizers to converge to a physically realizable material in ∼ 50 energy evaluations—far fewer than combinatorial optimization methods. Applied to Co–Cr–Ni–V oxides for the alkaline oxygen evolution reaction (OER), EAT leads to a final recommended composition of Co_0.19Cr_0.06V_0.31Ni_0.44O.