论文标题
部分可观测时空混沌系统的无模型预测
Building Robust Machine Learning Models for Small Chemical Science Data: The Case of Shear Viscosity
论文作者
论文摘要
剪切粘度虽然是所有液体的基本特性,但在计算上估计分子动力学模拟的计算昂贵。最近,机器学习(ML)方法已被用于在许多情况下增强分子模拟,从而显示出以相对廉价的方式估算粘度的希望。但是,当数据集的大小较小时,ML方法如粘度一样较小时面临着巨大的挑战。在这项工作中,我们训练多个ML模型,以预测Lennard-Jones(LJ)流体的剪切粘度,特别强调解决由小型数据集引起的问题。具体而言,研究了与模型选择,绩效估计和不确定性定量有关的问题。首先,我们表明,使用单个看不见的数据集的广泛使用的性能估计步骤显示了小数据集的广泛可变性。在这种情况下,可以使用交叉验证(CV)选择超参数(模型选择)的常见实践,以估算概括误差(性能估计)。我们比较了两个简单的简历程序,以便他们同时选择模型选择和性能估计的能力,并发现基于K折CV的过程显示出较低的错误估计差异。我们讨论绩效指标在培训和评估中的作用。最后,使用高斯工艺回归(GPR)和集合方法来估计单个预测的不确定性。 GPR的不确定性估计还用于构建适用性域,使用ML模型对本工作中生成的另一个小数据集提供了更可靠的预测。总体而言,这项工作中规定的程序共同为小型数据集提供了强大的ML模型。
Shear viscosity, though being a fundamental property of all liquids, is computationally expensive to estimate from equilibrium molecular dynamics simulations. Recently, Machine Learning (ML) methods have been used to augment molecular simulations in many contexts, thus showing promise to estimate viscosity too in a relatively inexpensive manner. However, ML methods face significant challenges like overfitting when the size of the data set is small, as is the case with viscosity. In this work, we train several ML models to predict the shear viscosity of a Lennard-Jones (LJ) fluid, with particular emphasis on addressing issues arising from a small data set. Specifically, the issues related to model selection, performance estimation and uncertainty quantification were investigated. First, we show that the widely used performance estimation procedure of using a single unseen data set shows a wide variability on small data sets. In this context, the common practice of using Cross validation (CV) to select the hyperparameters (model selection) can be adapted to estimate the generalization error (performance estimation) as well. We compare two simple CV procedures for their ability to do both model selection and performance estimation, and find that k-fold CV based procedure shows a lower variance of error estimates. We discuss the role of performance metrics in training and evaluation. Finally, Gaussian Process Regression (GPR) and ensemble methods were used to estimate the uncertainty on individual predictions. The uncertainty estimates from GPR were also used to construct an applicability domain using which the ML models provided more reliable predictions on another small data set generated in this work. Overall, the procedures prescribed in this work, together, lead to robust ML models for small data sets.