提出自洽电荷机器学习势的统一框架,揭示现有模型本质与局限。
Design Space of Self--Consistent Electrostatic Machine Learning Interatomic Potentials
- 将电荷模型视为密度泛函理论的粗粒化近似,明确其物理意义
- 在金属-水界面和二氧化硅空位上验证,现有方法在电荷响应上失败
- 构建可对比的自洽模型,为未来设计提供清晰路径
机器学习原子间势(MLIPs)已成为原子模拟中的常用工具。长期以来,主流架构基于短程原子能量贡献,局部性假设仍存在于许多现代基础模型中。尽管该方法在多数场景下高效准确,但在长程静电、电荷转移或诱导极化起关键作用的体系中存在固有局限。近年来,已有研究提出包含静电效应的扩展模型,从局部预测原子电荷到自洽模型不等。虽在特定案例中取得成功,但其基本假设与根本局限尚不清晰。本文提出一种将静电纳入MLIP的框架,将现有模型视为密度泛函理论(DFT)的粗粒化近似。这一视角显式揭示了近似项,澄清了学习量的物理含义,并揭示了多个先前模型间的联系与等价性。基于此形式化,我们识别出定义更广泛自洽电荷MLIP设计空间的关键设计选择。通过在MACE架构中实现共享电荷密度表示,我们构建了可控制比较的不同方法。最后,在两个典型测试案例上评估:金属-水界面,考察导体与绝缘体系统的对比电荷响应;以及二氧化硅中的带电空位。结果凸显现有方法的局限,并证明更表达力的自洽模型对解决失败至关重要。
原文摘要 · Abstract (English)
Machine learning interatomic potentials (MLIPs) have become widely used tools in atomistic simulations. For much of the history of this field, the most commonly employed architectures were based on short-ranged atomic energy contributions, and the assumption of locality still persists in many modern foundation models. While this approach has enabled efficient and accurate modelling for many use cases, it poses intrinsic limitations for systems where long-range electrostatics, charge transfer, or induced polarization play a central role. A growing body of work has proposed extensions that incorporate electrostatic effects, ranging from locally predicted atomic charges to self-consistent models. While these models have demonstrated success for specific examples, their underlying assumptions, and fundamental limitations are not yet well understood. In this work, we present a framework for treating electrostatics in MLIPs by viewing existing models as coarse-grained approximations to density functional theory (DFT). This perspective makes explicit the approximations involved, clarifies the physical meaning of the learned quantities, and reveals connections and equivalences between several previously proposed models. Using this formalism, we identify key design choices that define a broader design space of self-consistent electrostatic MLIPs. We implement salient points in this space using the MACE architecture and a shared representation of the charge density, enabling controlled comparisons between different approaches. Finally, we evaluate these models on two instructive test cases: metal-water interfaces, which probe the contrasting electrostatic response of conducting and insulating systems, and charged vacancies in silicon dioxide. Our results highlight the limitations of existing approaches and demonstrate how more expressive self-consistent models are needed to resolve failures.
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