Electrostatic Phenomenology Benchmarks for Machine-Learned Interatomic Potentials in Electrochemistry: Beyond the Energy-Force Metric

Abstract

Accurate treatment of long-range interactions in machine learning interatomic potentials (MLIPs) is essential for electrochemical simulations. However, aggregate energy and force errors alone are insufficient to establish an MLIP's physical accuracy since they do not detect qualitative inconsistencies in the model such as the prediction of image-charge attraction, dielectric screening, or charge transfer. We introduce a benchmark suite EPhEct (Electrostatic Phenomena for Electrochemistry) of focused test cases designed to evaluate MLIPs on electrochemically relevant physical phenomena. The tests probe for image-charge attraction at a metal electrode, the splitting between longitudinal and transverse optical phonons as a probe of ionic and electronic screening, the dipole moment of interfacial water, and Fermi-level pinning during ion discharge. These tests establish a qualitative diagnostic routine complementary to aggregate energy-force metrics.