Pulido Angeles, Chen Linjiang, Kaczorowski Tomasz, Holden Daniel, Little Marc A, Chong Samantha Y, Slater Benjamin J, McMahon David P, Bonillo Baltasar, Stackhouse Chloe J, Stephenson Andrew, Kane Christopher M, Clowes Rob, Hasell Tom, Cooper Andrew I, Day Graeme M
Computational Systems Chemistry, School of Chemistry, University of Southampton, Southampton, UK.
Department of Chemistry, University of Liverpool, Liverpool, UK.
Nature. 2017 Mar 30;543(7647):657-664. doi: 10.1038/nature21419. Epub 2017 Mar 22.
Molecular crystals cannot be designed in the same manner as macroscopic objects, because they do not assemble according to simple, intuitive rules. Their structures result from the balance of many weak interactions, rather than from the strong and predictable bonding patterns found in metal-organic frameworks and covalent organic frameworks. Hence, design strategies that assume a topology or other structural blueprint will often fail. Here we combine computational crystal structure prediction and property prediction to build energy-structure-function maps that describe the possible structures and properties that are available to a candidate molecule. Using these maps, we identify a highly porous solid, which has the lowest density reported for a molecular crystal so far. Both the structure of the crystal and its physical properties, such as methane storage capacity and guest-molecule selectivity, are predicted using the molecular structure as the only input. More generally, energy-structure-function maps could be used to guide the experimental discovery of materials with any target function that can be calculated from predicted crystal structures, such as electronic structure or mechanical properties.
分子晶体无法像宏观物体那样进行设计，因为它们并非按照简单直观的规则进行组装。其结构源于多种弱相互作用的平衡，而非金属有机框架和共价有机框架中那种强大且可预测的键合模式。因此，假定拓扑结构或其他结构蓝图的设计策略往往会失败。在这里，我们将计算晶体结构预测和性质预测相结合，构建能量-结构-功能图，以描述候选分子可能具有的结构和性质。利用这些图，我们识别出一种高度多孔的固体，它是迄今为止报道的分子晶体中密度最低的。仅以分子结构作为唯一输入，就能预测该晶体的结构及其物理性质，如甲烷储存容量和客体分子选择性。更一般地说，能量-结构-功能图可用于指导实验发现具有任何可从预测晶体结构计算得出的目标功能的材料，如电子结构或机械性能。
