发表机构
University of Warwick; École Polytechnique Fédérale de Lausanne; University of Vienna; Georg-August University, Göttingen; Max-Planck-Institute for Multidisciplinary Sciences（华威大学; 洛桑联邦理工学院; 维也纳大学; 哥廷根乔治-奥古斯特大学; 马克斯·普朗克多学科科学研究所）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究评估三种长程机器学习原子间势（MACE-POLAR、MACE-LES、LOREM）与短程基线模型在SrTiO$_3$缺陷能量学中的表现，通过从合成到真实系统的递进基准，验证其捕捉长程静电相互作用及预测氧空位迁移势垒的能力。
AI 中文摘要
机器学习原子间势（MLIPs）近年来发展迅速，但大多数模型本质上是半局域的，忽略了长程静电相互作用。为解决这一局限性，越来越多的长程模型应运而生，但系统性地比较它们在物理现实系统上的性能的基准研究仍然稀缺。在本工作中，我们评估了三种长程MLIPs——MACE-POLAR、MACE-LES和LOREM，并与短程基线MACE模型进行对比，考察它们捕捉长程库仑相互作用的能力，从理想化的合成点电荷系统逐步推进到基于第一性原理数据的真实晶体结构。这一递进过程使我们能够从DFT总能量中存在的多种竞争性能量贡献（如介电屏蔽和交换关联）中，隔离出模型学习静电相互作用的能力。作为一个物理动机明确的基准系统，我们聚焦于具有Sr-O肖特基空位对的钛酸锶SrTiO$_3$，在该材料中长程电荷相互作用起着核心作用，并且是研究带电极化子及其他电子和光学性质的自然跳板。基于此基准，我们进一步研究了在存在Sr-O肖特基对的情况下氧空位的迁移，使用爬坡图像微推弹性带计算和分子动力学来获得作为空位对间距函数的激活势垒，为每个模型捕捉控制缺陷输运的静电效应的能力提供了进一步的外推测试。
英文摘要
Machine learning interatomic potentials (MLIPs) have advanced rapidly in recent years, yet the majority of models remain semilocal in nature and neglect long-range electrostatic interactions. A growing number of long-range models have emerged to address this limitation, but systematic benchmarks comparing their performance on physically realistic systems remain scarce. In this work, we assess three long-range MLIPs -- MACE-POLAR, MACE-LES, and LOREM, against a short-range baseline MACE model, on their ability to capture long-range Coulombic interactions, progressing from idealised synthetic point-charge systems to first-principles data on realistic crystal structures. This progression allows us to isolate model's capability to learn electrostatic interactions from the many competing energy contributions, such as dielectric screening and exchange-correlation, that are present in DFT total energies. As a physically motivated benchmark system, we focus on strontium titanate SrTiO$_3$ with Sr--O Schottky vacancy pairs, a material in which long-range charge interactions play a central role and which serves as a natural stepping stone towards the study of charged polarons and other electronic and optical properties. Building on this benchmark, we further examine oxygen vacancy migration in the presence of the Sr--O Schottky pair, using climbing-image nudged elastic band calculations and molecular dynamics to obtain activation barriers as a function of the vacancy pair separation, providing further extrapolation test of each model's ability to capture the electrostatic effects that govern defect transport.
Comments20 pages, 13 figures
