A benchmark suite of focused test cases designed to evaluate MLIPs on electrochemically relevant physical phenomena and establish a qualitative diagnostic routine complementary to aggregate energy-force metrics is introduced.
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.
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Machine-learned interatomic potentials (MLIPs) have emerged as a strategy to accelerate molecular simulations, offering the promise of quantum chemical accuracy at a cost close to that of classical force fields. They are commonly trained on reference data obtained at the DFT level, which is itself a sufficiently afford...
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The role of atomistic simulation in battery research is examined, especially in the context of the capabilities afforded by MLIPs, and their advantages and trade-offs relative to ab initio methods are outlined.
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(English) Understanding how atomic-scale mechanisms govern ionic and electronic transport is crucial for the design of next-generation energy materials. Here, we combine first-principles simulations and machine-learning techniques to provide predictive and transferable approaches for modelling and understanding at the...
Accurate interpretation of X-ray photoelectron spectroscopy (XPS) in complex environments remains a longstanding challenge, as core-level binding energies (BEs) reflect a convolution of local chemical bonding and long-range electrostatic effects. In heterogeneous systems such as electrochemical interfaces and solvated...
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