Bigi Filippo, Pozdnyakov Sergey N, Ceriotti Michele
Laboratory of Computational Science and Modeling, Institut des Matériaux, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland.
J Chem Phys. 2024 Jul 28;161(4). doi: 10.1063/5.0208746.
Machine-learning models based on a point-cloud representation of a physical object are ubiquitous in scientific applications and particularly well-suited to the atomic-scale description of molecules and materials. Among the many different approaches that have been pursued, the description of local atomic environments in terms of their discretized neighbor densities has been used widely and very successfully. We propose a novel density-based method, which involves computing "Wigner kernels." These are fully equivariant and body-ordered kernels that can be computed iteratively at a cost that is independent of the basis used to discretize the density and grows only linearly with the maximum body-order considered. Wigner kernels represent the infinite-width limit of feature-space models, whose dimensionality and computational cost instead scale exponentially with the increasing order of correlations. We present several examples of the accuracy of models based on Wigner kernels in chemical applications, for both scalar and tensorial targets, reaching an accuracy that is competitive with state-of-the-art deep-learning architectures. We discuss the broader relevance of these findings to equivariant geometric machine-learning.
基于物理对象点云表示的机器学习模型在科学应用中无处不在,尤其适用于分子和材料的原子尺度描述。在众多已采用的不同方法中,根据离散化的邻域密度来描述局部原子环境已被广泛且非常成功地应用。我们提出了一种新颖的基于密度的方法,该方法涉及计算“维格纳核”。这些是完全等变且按体序排列的核,可以以与用于离散化密度的基无关的成本进行迭代计算,并且仅随着所考虑的最大体序线性增长。维格纳核代表了特征空间模型的无限宽度极限,而特征空间模型的维度和计算成本却随着相关阶数的增加呈指数增长。我们给出了基于维格纳核的模型在化学应用中的几个准确性示例,包括标量和张量目标,其准确性与当前最先进的深度学习架构具有竞争力。我们讨论了这些发现与等变几何机器学习的更广泛相关性。