论文标题

关于原子结构表示的完整性

On the Completeness of Atomic Structure Representations

论文作者

Pozdnyakov, Sergey N., Willatt, Michael J., Bartók, Albert P., Ortner, Christoph, Csányi, Gábor, Ceriotti, Michele

论文摘要

多体描述符被广泛用于代表原子学间潜能的构建原子环境,并且更广泛地用于原子结构上的拟合,分类和嵌入任务。人们普遍认为,三体描述符独特地指定原子的环境,直至类似原子的旋转和置换。我们对这种信念产生了几个反样本,结果是,使用3(或4)个体功能的任何分类器,回归或嵌入模型都将为不同的配置提供相同的结果。将全球属性(例如总能量)撰写为许多以原子为中心的贡献的总和减轻了这种基本缺陷的影响 - 解释了当前的“机器学习”力场的成功。我们预计随着所需准确性的提高,会出现的问题,并提出潜在的解决方案。

Many-body descriptors are widely used to represent atomic environments in the construction of machine learned interatomic potentials and more broadly for fitting, classification and embedding tasks on atomic structures. It was generally believed that 3-body descriptors uniquely specify the environment of an atom, up to a rotation and permutation of like atoms. We produce several counterexamples to this belief, with the consequence that any classifier, regression or embedding model for atom-centred properties that uses 3 (or 4)-body features will incorrectly give identical results for different configurations. Writing global properties (such as total energies) as a sum of many atom-centred contributions mitigates, but does not eliminate, the impact of this fundamental deficiency -- explaining the success of current "machine-learning" force fields. We anticipate the issues that will arise as the desired accuracy increases, and suggest potential solutions.

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