Understanding molecular adsorption on surfaces underpins many problems in chemistry and materials science. Accurately and efficiently describing the adsorption has been a challenging task for first-principles methods as the process can involve both short-range chemical bond formations and long-range physical interactions, e.g., the van der Waals (vdW) interaction. Density functional theory presents an appealing choice for modeling adsorption reactions, though calculations with many exchange correlation density functional approximations struggle to accurately describe both chemical and physical molecular adsorptions. Here, we propose an efficient density functional approximation that is accurate for both chemical and physical adsorption by concurrently optimizing its semilocal component and the long-range vdW correction against the prototypical adsorption CO/Pt(111) and Ar2 binding energy curve. The resulting functional opens the door to accurate and efficient modeling of general molecular adsorption.
@article{arxiv.2410.11248,
title = {Towards chemical accuracy for chemi- and physisorption with an efficient density functional},
author = {Manish Kothakonda and Ruiqi Zhang and Jinliang Ning and James Furness and Abhirup Patra and Qing Zhao and Jianwei Sun},
journal= {arXiv preprint arXiv:2410.11248},
year = {2025}
}