论文标题

通过第一原理和深度学习熔化温度预测

Melting temperature prediction via first principles and deep learning

论文作者

Hong, Qi-Jun

论文摘要

熔化是一个高温过程,需要大量的配置空间采样,从而使熔化的温度预测在计算上非常昂贵且具有挑战性。在过去的几年中,我建立了两种解决这一挑战的方法,一种是通过直接密度功能理论(DFT)分子动力学(MD)模拟,另一种是通过深度学习图神经网络。 DFT方法基于对小型固定共存MD模拟的统计分析。它消除了在快速加热方法中具有亚稳态过热固体的风险,同时也大大降低了相对于传统的大规模共存方法的计算机成本。既准确又有效(以每种材料几天的速度)被认为是直接DFT熔化温度计算的最佳方法之一。深度学习方法基于图形神经网络,可有效处理化学公式中的排列不变性,从而大大提高效率并降低成本。以每种材料毫秒的速度,该模型非常快,同时适度准确,尤其是在数据集扩展的组成空间内。我已经将这两种方法实施到自动化的计算机代码软件包中,使其公开可用并免费下载。 DFT和深度学习方法相互互补,因此它们可以很好地整合到融化温度预测的框架中。我演示了将方法应用于材料设计和发现高点点材料的示例。

Melting is a high temperature process that requires extensive sampling of configuration space, thus making melting temperature prediction computationally very expensive and challenging. Over the past few years, I have built two methods to address this challenge, one via direct density functional theory (DFT) molecular dynamics (MD) simulations and the other via deep learning graph neural networks. The DFT approach is based on statistical analysis of small-size solid-liquid coexistence MD simulations. It eliminates the risk of metastable superheated solid in the fast-heating method, while also significantly reducing the computer cost relative to the traditional large-scale coexistence method. Being both accurate and efficient (at the speed of several days per material), it is considered as one of the best methods for direct DFT melting temperature calculation. The deep learning method is based on graph neural networks that effectively handles permutation invariance in chemical formula, which drastically improves efficiency and reduces cost. At the speed of milliseconds per material, the model is extremely fast, while being moderately accurate, especially within the composition space expanded by the dataset. I have implemented both methods into automated computer code packages, making them publicly available and free to download. The DFT and deep learning methods are highly complementary to each other, and hence they can be potentially well integrated into a framework for melting temperature prediction. I demonstrated examples of applying the methods to materials design and discovery of high-melting-point materials.

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