English

Delta-learned force fields for nonbonded interactions: Addressing the strength mismatch between covalent-nonbonded interaction for global models

Chemical Physics 2025-11-05 v1 Materials Science Machine Learning Computational Physics

Abstract

Noncovalent interactions--vdW dispersion, hydrogen/halogen bonding, ion-π\pi, and π\pi-stacking--govern structure, dynamics, and emergent phenomena in materials and molecular systems, yet accurately learning them alongside covalent forces remains a core challenge for machine-learned force fields (MLFFs). This challenge is acute for global models that use Coulomb-matrix (CM) descriptors compared under Euclidean/Frobenius metrics in multifragment settings. We show that the mismatch between predominantly covalent force labels and the CM's overrepresentation of intermolecular features biases single-model training and degrades force-field fidelity. To address this, we introduce \textit{Δ\Delta-sGDML}, a scale-aware formulation within the sGDML framework that explicitly decouples intra- and intermolecular physics by training fragment-specific models alongside a dedicated binding model, then composing them at inference. Across benzene dimers, host-guest complexes (C60_{60}@buckycatcher, NO3_3^-@i-corona[6]arene), benzene-water, and benzene-Na+^+, \mbox{Δ\Delta-sGDML} delivers consistent gains over a single global model, with fragment-resolved force-error reductions up to \textbf{75\%}, without loss of energy accuracy. Furthermore, molecular-dynamics simulations further confirm that the Δ\Delta-model yields a reliable force field for C60_{60}@buckycatcher, producing stable trajectories across a wide range of temperatures (10-400~K), unlike the single global model, which loses stability above \sim200~K. The method offers a practical route to homogenize per-fragment errors and recover reliable noncovalent physics in global MLFFs.

Keywords

Cite

@article{arxiv.2511.01913,
  title  = {Delta-learned force fields for nonbonded interactions: Addressing the strength mismatch between covalent-nonbonded interaction for global models},
  author = {Leonardo Cázares-Trejo and Marco Loreto-Silva and Huziel E. Sauceda},
  journal= {arXiv preprint arXiv:2511.01913},
  year   = {2025}
}

Comments

12 pages, 8 figures

R2 v1 2026-07-01T07:19:56.093Z