论文标题

分子动力学和采样的不确定性估计

Uncertainty estimation for molecular dynamics and sampling

论文作者

Imbalzano, Giulio, Zhuang, Yongbin, Kapil, Venkat, Rossi, Kevin, Engel, Edgar A., Grasselli, Federico, Ceriotti, Michele

论文摘要

机器学习模型已成为一种非常有效的策略,用于避开耗时的电子结构计算,从而可以准确地模拟更大的尺寸,时间尺度和复杂性。鉴于这些模型的插值性质,预测的可靠性取决于相位空间中的位置,并且至关重要的是,从模型训练期间包含的有限参考结构数量得出的误差估算至关重要。当使用机器学习电位对有限温度集合进行采样时,单个配置的不确定性转化为热力学平均值的错误,并在模拟进入先前未开发的区域时提供了准确性丧失的指示。在这里,我们讨论如何将不确定性定量与基线能量模型一起使用,或者是更坚固的原子间潜力,以获得更多的弹性模拟并支持主动学习策略。此外,我们引入了一种直接的重新呼叫方案,该方案可以估算从长轨迹中提取的热力学平均值的不确定性。我们提出了涵盖不同类型的结构和热力学特性的例子,以及与水和液体壳一样多样化的系统。

Machine learning models have emerged as a very effective strategy to sidestep time-consuming electronic-structure calculations, enabling accurate simulations of greater size, time scale and complexity. Given the interpolative nature of these models, the reliability of predictions depends on the position in phase space, and it is crucial to obtain an estimate of the error that derives from the finite number of reference structures included during the training of the model. When using a machine-learning potential to sample a finite-temperature ensemble, the uncertainty on individual configurations translates into an error on thermodynamic averages, and provides an indication for the loss of accuracy when the simulation enters a previously unexplored region. Here we discuss how uncertainty quantification can be used, together with a baseline energy model, or a more robust although less accurate interatomic potential, to obtain more resilient simulations and to support active-learning strategies. Furthermore, we introduce an on-the-fly reweighing scheme that makes it possible to estimate the uncertainty in the thermodynamic averages extracted from long trajectories. We present examples covering different types of structural and thermodynamic properties, and systems as diverse as water and liquid gallium.

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