Accurate Modeling of Organic Molecular Crystals by Dispersion-Corrected Density Functional Tight Binding (DFTB)
Accurate Modeling of Organic Molecular Crystals by Dispersion-Corrected Density Functional Tight Binding (DFTB)
复制标题
DOI：
10.1021/jz500755u
复制
发表时间：
2014-06-05
影响因子：
5.7
通讯作者：
Grimme, Stefan
中科院分区：
文献类型：
--
作者：
Brandenburg, Jan Gerit;Grimme, Stefan
有机晶体结构预测的宏伟目标对理论方法的准确性和效率提出了挑战。色散校正密度泛函理论（DFT-D）原则上是适用的，但计算要求，例如，计算大量的多晶型物，太高。在这里，我们证明了这项任务可以通过色散校正的密度泛函紧束缚（DFTB）方法进行。与D3校正的半经验哈密顿量可以准确和有效地模拟固相和气相分子间和分子内的相互作用，速度比DFT-D提高2个数量级。各种数据库的相互作用（晶格）能量的平均绝对偏差通常为2-3 kcal/mol（10-20%），即仅比DFT-D的平均绝对偏差大约两倍。对于零点声子能量，
The ambitious goal of organic crystal structure prediction challenges theoretical methods regarding their accuracy and efficiency. Dispersion-corrected density functional theory (DFT-D) in principle is applicable, but the computational demands, for example, to compute a huge number of polymorphs, are too high. Here, we demonstrate that this task can be carried out by a dispersion-corrected density functional tight binding (DFTB) method. The semiempirical Hamiltonian with the D3 correction can accurately and efficiently model both solid- and gas-phase inter- and intramolecular interactions at a speed up of 2 orders of magnitude compared to DFT-D. The mean absolute deviations for interaction (lattice) energies for various databases are typically 2-3 kcal/mol (10-20%), that is, only about two times larger than those for DFT-D. For zero-point phonon energies, small deviations of