Banerjee Atreyee, Jasrasaria Dipti, Niblett Samuel P, Wales David J
Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom.
Max Planck Institute for Polymer Research, 55128 Mainz, Germany.
J Phys Chem A. 2021 May 6;125(17):3776-3784. doi: 10.1021/acs.jpca.1c00903. Epub 2021 Apr 21.
Organic molecules can be stable in distinct crystalline forms, known as polymorphs, which have significant consequences for industrial applications. Here, we predict the polymorphs of crystalline benzene computationally for an accurate anisotropic model parametrized to reproduce electronic structure calculations. We adapt the basin-hopping global optimization procedure to the case of crystalline unit cells, simultaneously optimizing the molecular coordinates and unit cell parameters to locate multiple low-energy structures from a variety of crystal space groups. We rapidly locate all the well-established experimental polymorphs of benzene, each of which corresponds to a single local energy minimum of the model. Our results show that basin-hopping can be both an efficient and effective tool for polymorphic crystal structure prediction, requiring no experimental knowledge of cell parameters or symmetry.
有机分子可以以不同的晶体形式稳定存在，即多晶型物，这对工业应用具有重大影响。在此，我们通过计算预测结晶苯的多晶型物，以获得一个精确的各向异性模型参数化，用于重现电子结构计算。我们将盆地跳跃全局优化程序应用于晶体晶胞的情况，同时优化分子坐标和晶胞参数，以便从各种晶体空间群中定位多个低能量结构。我们快速定位了苯所有已确定的实验多晶型物，每一种都对应于该模型的一个局部能量最小值。我们的结果表明，盆地跳跃可以成为多晶型晶体结构预测的一种高效且有效的工具，无需关于晶胞参数或对称性的实验知识。
