Supporting Data for: A Multimer Embedding Approach for Molecular Crystals up to Harmonic Vibrational Properties

Accurate calculations of molecular crystals would be crucial for drug design and crystal engineering. However, periodic high-level density functional calculations using hybrid functionals are often prohibitively expensive for relevant systems. Therefore, these expensive periodic calculations are sometimes circumvented by the usage of quantum-mechanical embedding methods, in which for instance the periodic calculation is only performed at a lower-cost level and then monomer energies and dimer interactions are replaced by those of the higher-level method. Herein, we extend upon such a multimer embedding approach to enable energy corrections for trimer interactions and the calculation of harmonic vibrational properties up to the dimer level. We show that trimer interactions are crucial for accurately approximating lattice energies and might also be needed for a better description of lattice constants. Finally, vibrational properties are already very well captured at the dimer level.<br> This supporting dataset includes results of PBE0+MBD/light, PBE+MBD/light, and multimer embedding calculations for the X23 set of molecular crystals. See the included README.md file for more details. The related preprint can be found at https://doi.org/10.48550/arXiv.2209.02687.精准的分子晶体计算对于药物设计与晶体工程而言至关重要。然而，针对相关体系采用杂化泛函的周期性高精度密度泛函计算，其计算成本往往高得难以承受。为此，研究人员常采用量子力学嵌入方法来规避这类高成本的周期性计算：例如，先以低成本精度开展周期性计算，再将单体能量与二聚体相互作用替换为高精度方法的计算结果。本文中，我们对该类多聚体嵌入方法进行拓展，使其可用于三聚体相互作用的能量校正，以及至多二聚体层级的简谐振动特性计算。我们证实，三聚体相互作用对于精准近似晶格能量至关重要，同时也可能是更准确描述晶格常数的必要条件。最终，在二聚体层级即可很好地复现振动特性。 本配套数据集包含X23分子晶体集的PBE0+MBD/light、PBE+MBD/light以及多聚体嵌入计算结果。更多细节请参阅附带的README.md文件。相关预印本可访问https://doi.org/10.48550/arXiv.2209.02687获取。