Dittrich B, Connor L E, Fabbiani F P A, Piechon P
Novartis Campus, Novartis Pharma AG, Postfach, Basel CH-4002, Switzerland.
IUCrJ. 2024 May 1;11(Pt 3):347-358. doi: 10.1107/S2052252524002641.
Categorization underlies understanding. Conceptualizing solid-state structures of organic molecules with `archetype crystal structures' bridges established categories of disorder, polymorphism and solid solutions and is herein extended to special position and high-Z' structures. The concept was developed in the context of disorder modelling [Dittrich, B. (2021). IUCrJ, 8, 305-318] and relies on adding quantum chemical energy differences between disorder components to other criteria as an explanation as to why disorder - and disappearing disorder - occurs in an average structure. Part of the concept is that disorder, as probed by diffraction, affects entire molecules, rather than just the parts of a molecule with differing conformations, and the finding that an R·T energy difference between disorder archetypes is usually not exceeded. An illustrative example combining disorder and special positions is the crystal structure of oestradiol hemihydrate analysed here, where its space-group/subgroup relationship is required to explain its disorder of hydrogen-bonded hydrogen atoms. In addition, we show how high-Z' structures can also be analysed energetically and understood via archetypes: high-Z' structures occur when an energy gain from combining different rather than overall alike conformations in a crystal significantly exceeds R·T, and this finding is discussed in the context of earlier explanations in the literature. Twinning is not related to archetype structures since it involves macroscopic domains of the same crystal structure. Archetype crystal structures are distinguished from crystal structure prediction trial structures in that an experimental reference structure is required for them. Categorization into archetype structures also has practical relevance, leading to a new practice of disorder modelling in experimental least-squares refinement alluded to in the above-mentioned publication.
分类是理解的基础。用“原型晶体结构”对有机分子的固态结构进行概念化,架起了无序、多晶型和固溶体等既定类别的桥梁,本文将其扩展到特殊位置和高Z'结构。该概念是在无序建模的背景下发展起来的[迪特里希,B.(2021年)。《IUCrJ》,8,305 - 318],它依赖于将无序组分之间的量子化学能量差添加到其他标准中,以解释为什么无序——以及无序的消失——会出现在平均结构中。该概念的一部分是,通过衍射探测到的无序会影响整个分子,而不仅仅是具有不同构象的分子部分,并且发现无序原型之间的R·T能量差通常不会被超过。一个结合了无序和特殊位置的示例是本文分析的雌二醇半水合物的晶体结构,其中需要其空间群/子群关系来解释其氢键合氢原子的无序。此外,我们展示了如何通过原型对高Z'结构进行能量分析和理解:当晶体中组合不同而非总体相似的构象所获得的能量显著超过R·T时,就会出现高Z'结构,并且在文献中早期解释的背景下讨论了这一发现。孪晶与原型结构无关,因为它涉及相同晶体结构的宏观畴。原型晶体结构与晶体结构预测试验结构的区别在于它们需要一个实验参考结构。分类为原型结构也具有实际意义,导致了上述出版物中提到的实验最小二乘精修中无序建模的新实践。