论文标题

自动发现铝的强大原子间潜力

Automated discovery of a robust interatomic potential for aluminum

论文作者

Smith, Justin S., Nebgen, Benjamin, Mathew, Nithin, Chen, Jie, Lubbers, Nicholas, Burakovsky, Leonid, Tretiak, Sergei, Nam, Hai Ah, Germann, Timothy, Fensin, Saryu, Barros, Kipton

论文摘要

分子动力学模拟的准确性取决于用于产生力的原子间潜能。黄金标准将是第一原理量子力学(QM)计算,但是在大型模拟尺度上,它们变得过于昂贵。基于机器学习(ML)的潜力旨在以大幅降低的计算成本忠实地模仿QM。 ML潜力的准确性和鲁棒性主要受培训数据集的质量和多样性的限制。使用主动学习原理(AL),我们提出了一种高度自动化的数据集构造方法。该策略是利用正在开发的ML潜力进行采样新的原子配置,并且每当达到ML不确定性足够大的配置时,收集新的QM数据。在这里,我们试图突破自动化的限制,从可能的过程中删除尽可能多的专业知识。所有抽样均使用最初无序的配置开始的MD模拟进行,并通过随时间变化的应用温度驱动的非平衡动力学进行。我们通过建立铝(Ani-al)的ML潜力来证明这种方法。经过多次迭代,Ani-Al教会自己预测诸如熔体中的径向分布函数,液态固体共存曲线以及缺陷能和屏障等晶体特性。为了证明可传递性,我们执行130万个原子冲击模拟,并表明Ani Al预测与从非平衡动力学采样的局部原子环境的DFT计算非常吻合。有趣的是,在AL培训数据集中,震惊中出现的配置似乎已经很好地采样了,我们以视觉上的方式说明了。

Accuracy of molecular dynamics simulations depends crucially on the interatomic potential used to generate forces. The gold standard would be first-principles quantum mechanics (QM) calculations, but these become prohibitively expensive at large simulation scales. Machine learning (ML) based potentials aim for faithful emulation of QM at drastically reduced computational cost. The accuracy and robustness of an ML potential is primarily limited by the quality and diversity of the training dataset. Using the principles of active learning (AL), we present a highly automated approach to dataset construction. The strategy is to use the ML potential under development to sample new atomic configurations and, whenever a configuration is reached for which the ML uncertainty is sufficiently large, collect new QM data. Here, we seek to push the limits of automation, removing as much expert knowledge from the AL process as possible. All sampling is performed using MD simulations starting from an initially disordered configuration, and undergoing non-equilibrium dynamics as driven by time-varying applied temperatures. We demonstrate this approach by building an ML potential for aluminum (ANI-Al). After many AL iterations, ANI-Al teaches itself to predict properties like the radial distribution function in melt, liquid-solid coexistence curve, and crystal properties such as defect energies and barriers. To demonstrate transferability, we perform a 1.3M atom shock simulation, and show that ANI-Al predictions agree very well with DFT calculations on local atomic environments sampled from the nonequilibrium dynamics. Interestingly, the configurations appearing in shock appear to have been well sampled in the AL training dataset, in a way that we illustrate visually.

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