发表机构
MPI for the Structure and Dynamics of Matter; Department of Chemistry, University of York; Physicochimie des Électrolytes et Nanosystèmes Interfaciaux, Sorbonne Université, CNRS; Institute of Inorganic Chemistry, RWTH Aachen University; Laboratoire de physique de L’École normale supérieure de Paris, CNRS, ENS & Université PSL, Sorbonne Université, Université de Paris; Yusuf Hamied Department of Chemistry, Cambridge University（物质结构与动力学马普研究所; 约克大学化学系; 索邦大学CNRS界面电解质与纳米系统物理化学研究所; 亚琛工业大学无机化学研究所; 巴黎高等师范学院CNRS实验室、ENS与PSL大学、索邦大学、巴黎大学; 剑桥大学优素福·哈米德化学系）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
SALTED是开源Python机器学习程序，基于原子坐标预测分子与材料电子密度，可对接主流电子结构程序，在小数据场景高效，能学习电场响应，已用于极化计算等多类研究。
AI 中文摘要
SALTED提供了一个开源Python包，用于基于输入的原子坐标和种类，对分子和凝聚相体系中的量子力学电子密度$n(\mathbf{r})$进行机器学习建模。该程序采用电子密度的线性原子中心分解，使其在具有相似化学环境的不同原子构型间具有高度可迁移性。由于这一表示选择，SALTED可自然地与基于原子轨道的最先进电子结构程序（即CP2K、FHI-aims和PySCF）对接，可从这些程序生成参考电子密度数据并用于训练模型。其学习算法基于高斯过程回归的对称自适应扩展，使SALTED在小数据 regime 中效率极高。得益于矢量场核函数的实现，SALTED还可学习电子密度对施加电场的一阶响应$\partial n(\mathbf{r})/\partial \mathbf{E}$。SALTED在计算工作流中的应用已在多种场景中展现出实用性，包括极化矢量和极化率张量的计算、QM/MM分子动力学模拟中库仑力的精确评估，以及大规模二维材料的电子结构研究。
英文摘要
SALTED provides an open-source Python package for machine learning the quantum-mechanical electron density, $n(\mathbf{r})$, in molecular and condensed-phase systems based on input atomic coordinates and species. The program adopts a linear atom-centered decomposition of the electron density, which makes it highly transferable across diverse atomistic configurations sharing similar chemical environments. Because of this representation choice, SALTED is naturally interfaced with state-of-the-art electronic-structure programs based on atomic orbitals, namely CP2K, FHI-aims, and PySCF, from which reference electron-density data can be generated and used to train a model. The learning algorithm is based on a symmetry-adapted extension of Gaussian process regression, making SALTED especially efficient in small-data regimes. Thanks to the implementation of vector-field kernel functions, SALTED can also learn the first-order response of the electron density to applied electric fields, $\partial n(\mathbf{r})/\partial \mathbf{E}$. The application of SALTED within computational workflows has already shown its utility in a wide variety of contexts, including the calculation of polarization vectors and polarizability tensors, the accurate evaluation of Coulomb forces in QM/MM molecular-dynamics simulations, and electronic-structure studies of large-scale 2D materials.
Comments7 pages, 1 figure
