Goletto Linda, Giovannini Tommaso, Folkestad Sarai D, Koch Henrik
Department of Chemistry, Norwegian University of Science and Technology (NTNU), 7491 Trondheim, Norway.
Scuola Normale Superiore, Piazza dei Cavalieri 7, I-56126 Pisa, Italy.
Phys Chem Chem Phys. 2021 Feb 25;23(7):4413-4425. doi: 10.1039/d0cp06359b.
We investigate the coupling of different quantum-embedding approaches with a third molecular-mechanics layer, which can be either polarizable or non-polarizable. In particular, such a coupling is discussed for the multilevel families of methods, in which the system is divided into an active and an inactive orbital space. The computational cost of the resulting three-layer approaches is reduced by treating the long-range interactions at the classical level. The developed methods are tested by the calculation of excitation energies of molecular systems in aqueous solution, for which an atomistic description of the environment is crucial to correctly reproduce the specific solute-solvent interactions, such as hydrogen bonding. In particular, we present the results obtained for three different moieties - acrolein, pyridine and para-nitroaniline - showing that an almost perfect agreement with experimental data can be achieved when the relevant physico-chemical interactions are included in the modeling of the condensed phase.
我们研究了不同量子嵌入方法与第三分子力学层的耦合，该分子力学层可以是可极化的或不可极化的。特别地，针对多级方法族讨论了这种耦合，在多级方法中，系统被划分为活性和非活性轨道空间。通过在经典水平处理长程相互作用，降低了所得三层方法的计算成本。通过计算水溶液中分子系统的激发能对所开发的方法进行了测试，对于该系统，环境的原子描述对于正确再现特定的溶质 - 溶剂相互作用（如氢键）至关重要。特别地，我们展示了针对三种不同部分——丙烯醛、吡啶和对硝基苯胺——获得的结果，表明当在凝聚相建模中纳入相关物理化学相互作用时，可以实现与实验数据几乎完美的吻合。
