Generalized convex hull construction for materials discovery
Generalized convex hull construction for materials discovery
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DOI：
10.1103/physrevmaterials.2.103804
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发表时间：
2018-10-22
影响因子：
3.4
通讯作者：
Ceriotti, Michele
中科院分区：
文献类型：
--
作者：
Anelli, Andrea;Engel, Edgar A.;Ceriotti, Michele
寻找新的材料包括确定潜在的候选材料，并选择那些具有理想性能和易于合成的材料。例如，通过计算搜索或元素替换，生成大量潜在候选对象相对容易。然而，可合成化合物的鉴定是一个大海捞针的问题。传统上，筛选是基于凸壳结构的，它识别由特定热力学约束(如压力)稳定的结构，该结构是基于先前的实验证据或直觉选择的。我们引入了一个广义的凸壳框架，该框架依赖于数据驱动的坐标，并以一种公正的方式表示候选化合物的全部结构多样性。它的概率结构解决了输入结构数据中不可避免的不确定性，并提供了比输入(自由)能量更好的稳定性测量，例如，这也可以用于辅助实验晶体结构确定。它有效地识别了具有高概率可合成的候选对象，并提出了相关的实验可实现的限制条件，从而为确定可行的合成途径提供了一个亟需的起点。
Searching for novel materials involves identifying potential candidates and selecting those that have desirable properties and facile synthesis. It is relatively easy to generate large numbers of potential candidates, for instance, by computational searches or elemental substitution. The identification of synthesizable compounds, however, is a needle-in-a-haystack problem. Conventionally, the screening is based on a convex hull construction, which identifies structures stabilized by a particular thermodynamic constraint, such as pressure, chosen based on prior experimental evidence or intuition. We introduce a generalized convex hull framework that instead relies on data-driven coordinates, and represents the full structural diversity of the candidate compounds in an unbiased way. Its probabilistic construction addresses the inevitable uncertainty in input structure data and provides a superior measure of stability compared to the input (free) energies, that can, for instance, also be used to assist experimental crystal structure determination. It efficiently identifies candidates with high probabilities of being synthesizable and suggests the relevant experimentally realizable constraints, thereby providing a much needed starting point for the determination of viable synthetic pathways.