Kaplan F, Harding M E, Seiler C, Weigend F, Evers F, van Setten M J
Institute of Nanotechnology, Karlsruhe Institute of Technology , Campus North, D-76344 Karlsruhe, Germany.
Institute of Theoretical Physics, University of Regensburg , D-93040 Regensburg, Germany.
J Chem Theory Comput. 2016 Jun 14;12(6):2528-41. doi: 10.1021/acs.jctc.5b01238. Epub 2016 May 26.
We present the formalism and implementation of quasi-particle self-consistent GW (qsGW) and eigenvalue only quasi-particle self-consistent GW (evGW) adapted to standard quantum chemistry packages. Our implementation is benchmarked against high-level quantum chemistry computations (coupled-cluster theory) and experimental results using a representative set of molecules. Furthermore, we compare the qsGW approach for five molecules relevant for organic photovoltaics to self-consistent GW results (scGW) and analyze the effects of the self-consistency on the ground state density by comparing calculated dipole moments to their experimental values. We show that qsGW makes a significant improvement over conventional G0W0 and that partially self-consistent flavors (in particular evGW) can be excellent alternatives.
我们展示了适用于标准量子化学软件包的准粒子自洽GW（qsGW）和仅本征值准粒子自洽GW（evGW）的形式体系及实现方法。我们的实现方法以一组具有代表性的分子为对象，与高水平量子化学计算（耦合簇理论）和实验结果进行了基准测试。此外，我们将与有机光伏相关的五个分子的qsGW方法与自洽GW结果（scGW）进行了比较，并通过将计算得到的偶极矩与实验值相比较，分析了自洽性对基态密度的影响。我们表明，qsGW相对于传统的G0W0有显著改进，部分自洽形式（特别是evGW）可以是很好的替代方法。
