分子晶体光吸收谱的精确和有效计算：ROY多晶型的情况
Accurate and efficient computation of optical absorption spectra of molecular crystals: the case of the polymorphs of ROY
摘要：
在用第一性原理计算分子晶体的吸收光谱时，晶体环境对激发态的影响是非常重要的。然而，对于这样的系统，由于所涉及的相对大的系统尺寸，精确地描述激励的方法在计算上可能是禁止的。在这项工作中，我们展示了一种方法，使光学吸收光谱计算效率高，精度高。我们的方法是基于光谱弯曲方法成功地应用于溶剂中的分子。它涉及使用半局部TDDFT计算全分子晶体的超晶胞的吸收光谱，然后使用来自孤立二聚体的小规模半局部和混合TDDFT计算的变换来扭曲光谱。我们证明了这种方法的权力对三个多晶型的著名的彩色多晶型化合物ROY，并发现它优于小规模的混合TDDFT二聚体计算和大规模的半本地TDDFT超胞计算，当与实验相比。
英文摘要：
When calculating the optical absorption spectra of molecular crystals from first principles, the influence of the crystalline environment on the excitations is of significant importance. For such systems, however, methods to describe the excitations accurately can be computationally prohibitive due to the relatively large system sizes involved. In this work, we demonstrate a method that allows optical absorption spectra to be computed both efficiently and at high accuracy. Our approach is based on the spectral warping method successfully applied to molecules in solvent. It involves calculating the absorption spectrum of a supercell of the full molecular crystal using semi-local TDDFT, before warping the spectrum using a transformation derived from smaller-scale semi-local and hybrid TDDFT calculations on isolated dimers. We demonstrate the power of this method on three polymorphs of the well known colour polymorphic compound ROY, and find that it outperforms both small-scale hybrid TDDFT dimer calculations and large-scale semi-local TDDFT supercell calculations, when compared to experiment.
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