arXiv:2605.05746cond-mat.mtrl-scics.LG2026-05被引 4

用极化原子多极矩学习长程静电,提升机器学习势函数精度。

Polarizable atomic multipoles for learning long-range electrostatics

论文配图:Polarizable atomic multipoles for learning long-range electrostatics
图 1 · 摘自论文原文
  • 基于局部等变描述符预测环境依赖的电荷、偶极和四极矩
  • 无需直接监督即生成物理合理的电响应,准确预测红外与拉曼光谱
  • 适用于离子、极性及界面体系,适合材料模拟与光谱预测研究者

长程静电与极化仍是扩展机器学习原子间势(MLIPs)至离子、极性及界面体系的核心挑战。本文提出一种半局部框架,通过能量和力数据学习极化原子多极矩。局部等变描述符预测环境依赖的隐式单极、偶极和四极矩,残余非局域电荷转移与极化则通过非自洽线性响应模型捕捉。在四个不同基准测试及四种短程MLIP架构上,多极层次与响应项系统性提升势能面精度,尤其在长程效应关键的体系中增益显著。更重要的是,无需直接监督即可产生物理合理的电响应:学习到的隐式多极矩精确还原了玻恩有效电荷张量与红外光谱,与实验高度一致。偶极诱导扩展使模型可预测极化率,从而实现对体相水与混合钙钛矿MAPbI₃的半定量拉曼光谱建模,并成功再现水-空气界面表面特异性振动和频生成光谱的关键特征。在铁电HfO₂中,预测的电响应亦包含声子洛伦兹-托尔—弗兰克分裂与极化翻转行为。该可系统优化、物理透明的框架,使仅以标准能量与力标签训练的MLIP具备预测极化敏感可观测量的能力。

原文摘要 · Abstract (English)

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.

机器学习势极化多极矩光谱预测

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