We report the synthesis, structural characterization and magnetic properties of K3coronene, and demonstrate a computational screening workflow designed to accelerate the discovery of metal intercalated polycyclic aromatic hydrocarbon (PAH), a class of materials of interest following reports of superconductivity, but lacking demonstrated and understood characterised materials compositions. Coronene is identified as a suitable PAH candidate from a library of PAHs for potassium intercalation by computational screening of their electronic structure and of the void space in their crystal structures, targeting LUMO similarity to C60 and the availability of suitable sites to accommodate inserted cations. Convex hull calculations with energies from crystal structure prediction based on ion insertion into the identified void space of coronene suggest that the x = 3 composition in Kxcoronene is stable at 0 K, reinforcing the suitability of coronone for experimental investigation. Exploration of reaction conditions and compositions revealed that the mild reducing agent KH allows formation of K3coronene. The structure of K3coronene solved from synchrotron powder X-ray diffraction features extensive reorientation and associated disorder of coronene molecules compared with the parent pristine host. This is driven by K+ intercalation and occupation of sites both within and between the coronene stacks that are partially retained from the parent structure. This disruption of the host structure is greater when three cations are inserted per coronene than in reported metal PAH structures where the maximum ratio of cations to PAH is 2. Superconductivity is not observed, contrary to previous reports on Kxcoronene. The expected localised moment response of coronene3- is suppressed, which may be associated with the combination of extensive disorder and close coronene3- - coronene3- contacts.

中文翻译：

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由数据和计算引导的多次阳离子插入多环芳烃中


我们报告了 K3coronene 的合成、结构表征和磁性，并展示了一种计算筛选工作流程，旨在加速金属插层多环芳烃 （PAH） 的发现，这是一类在超导性报道之后感兴趣的材料，但缺乏证明和理解的表征材料组成。通过对多环芳烃的电子结构和晶体结构中的空隙空间进行计算筛选，从多环芳烃库中确定为适合用于钾嵌入的多环芳烃候选物，靶向 LUMO 与 C60 的相似性和容纳插入阳离子的合适位点的可用性。基于离子插入到已确定的冠烯空隙空间的晶体结构预测中能量的凸包计算表明，Kxcoronene 中的 x = 3 组成在 0 K 时稳定，这加强了冠酮对实验研究的适用性。对反应条件和组成的探索表明，温和的还原剂 KH 允许形成 K3 coronene。与母体原始宿主相比，由同步辐射粉末 X 射线衍射分离的 K3 coronene 的结构具有广泛的重新取向和相关的 coronene 分子无序。这是由 K+ 嵌入和占据冠烯堆栈内部和之间的位点驱动的，这些位点部分保留在母体结构中。当每个冠烯插入三个阳离子时，宿主结构的这种破坏比在已报道的金属 PAH 结构中更大，其中阳离子与 PAH 的最大比率为 2。没有观察到超导性，这与之前关于 Kxcoronene 的报道相反。 coronene3- 的预期局部时刻反应受到抑制，这可能与广泛的无序和密切的 coronene3- - coronene3- 接触有关。