在这项工作中,水晶密码,作者先前开发的用于在现有势能面(PES)函数中找到“空穴”以及合法的过渡态[JPCLett。11,6468(2020)],被重新设计为实时执行“直接动力学”类型的PES探索,以及自动构建新的PES功能。在所有这些情况下,与其他方法相比,Crystal的主要优势是它能够在全球范围内绘制PES,从而快速可靠地确定配置空间的最相关区域-即使维度相当大。这里,晶体用于生成密度泛函理论(DFT)或从头算点的均匀间隔网格,在相关区域上截断,然后可以用来:(a)精确地磨练PES特征,如最小值和过渡态,或(b)自动创建一个新的PES函数,通过插值。通过应用于三个分子系统来证明概念:水(H2O),(还原维)甲烷(CH4),和亚甲基亚胺(CH2NH)。
In this work, the Crystal code, developed previously by the authors to find \"holes\" as well as legitimate transition states in existing potential energy surface (PES) functions [JPC Lett. 11, 6468 (2020)], is retooled to perform on-the-fly \"direct dynamics\"-type PES explorations, as well as automatic construction of new PES functions. In all of these contexts, the chief advantage of Crystal over other methods is its ability to globally map the PES, thereby determining the most relevant regions of configuration space quickly and reliably-even when the dimensionality is rather large. Here, Crystal is used to generate a uniformly spaced grid of density functional theory (DFT) or ab initio points, truncated over the relevant regions, which can then be used to either: (a) hone in precisely on PES features such as minima and transition states, or; (b) create a new PES function automatically, via interpolation. Proof of concept is demonstrated via application to three molecular systems: water (H 2 O), (reduced-dimensional) methane (CH 4 ), and methylene imine (CH 2 NH).