4.7 Article

Robust relativistic many-body Green's function based approaches for assessing core ionized and excited states

期刊

JOURNAL OF CHEMICAL PHYSICS
卷 159, 期 4, 页码 -

出版社

AIP Publishing
DOI: 10.1063/5.0160265

关键词

-

向作者/读者索取更多资源

A two-component contour deformation (CD) based GW method is proposed to reduce the computational effort for assessing quasiparticle states. It achieves a significant reduction in computational scaling compared to the canonical CD-GW method. The efficiency improvement allows for benchmarking core ionized states and testing the performance of different density functional approximations as starting points for GW calculations. Furthermore, the core-valence separated Bethe-Salpeter equation (CVS-BSE) is introduced as a tool for probing core excited states.
A two-component contour deformation (CD) based GW method that employs frequency sampling to drastically reduce the computational effort when assessing quasiparticle states far away from the Fermi level is outlined. Compared to the canonical CD-GW method, computational scaling is reduced by an order of magnitude without sacrificing accuracy. This allows for an efficient calculation of core ionization energies. The improved computational efficiency is used to provide benchmarks for core ionized states, comparing the performance of 15 density functional approximations as Kohn-Sham starting points for GW calculations on a set of 65 core ionization energies of 32 small molecules. Contrary to valence states, GW calculations on core states prefer functionals with only a moderate amount of Hartree-Fock exchange. Moreover, modern ab initio local hybrid functionals are also shown to provide excellent generalized Kohn-Sham references for core GW calculations. Furthermore, the core-valence separated Bethe-Salpeter equation (CVS-BSE) is outlined. CVS-BSE is a convenient tool to probe core excited states. The latter is tested on a set of 40 core excitations of eight small inorganic molecules. Results from the CVS-BSE method for excitation energies and the corresponding absorption cross sections are found to be in excellent agreement with those of reference damped response BSE calculations.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.7
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据