Polarizable atomic multipoles for learning long-range electrostatics

Abstract:Long-range electrostatics and polarization remain central obstacles to extending machine learning interatomic potentials (MLIPs) to ionic, polar, and interfacial systems. Here we introduce a semi-local framework for learning electrostatics from energies and forces using polarizable atomic multipoles. Local equivariant descriptors predict environment-dependent latent monopoles, dipoles, and quadrupoles, while residual non-local charge transfer and polarization are captured by non-self-consistent linear response in induced charges and dipoles. Across four diverse benchmarks and four short-range MLIP architectures, the multipole hierarchy and response terms systematically improve potential energy surface accuracy, with the largest gains in systems where long-range effects are essential. More importantly, physically meaningful electrical responses emerge without direct supervision. The learned latent multipoles yield accurate Born effective charge tensors and infrared spectra in close agreement with experiments. The induced-dipole extension introduces new capabilities: it predicts polarizabilities and thereby enables semi-quantitative Raman spectra for bulk water and hybrid MAPbI$_3$ perovskite, as well as the essential features of the surface-specific vibrational sum-frequency generation spectrum at the water-air interface. In ferroelectric HfO$_2$, the predicted electrical response also captures LO-TO splitting and polarization switching. This systematically improvable, physically transparent framework enables MLIPs trained on standard energy and force labels to predict polarization-sensitive observables.

Materials Science (cond-mat.mtrl-sci); Machine Learning (cs.LG); Chemical Physics (physics.chem-ph); Computational Physics (physics.comp-ph)

arXiv:2605.05746 [cond-mat.mtrl-sci]

(or arXiv:2605.05746v2 [cond-mat.mtrl-sci] for this version)

https://doi.org/10.48550/arXiv.2605.05746 Focus to learn more arXiv-issued DOI via DataCite

Supplementary_Information.pdf

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