Optimally tuned starting point for single-shot GW calculations of solids
Optimally tuned starting point for single-shot GW calculations of solids
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DOI：
10.1103/physrevmaterials.6.053802
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发表时间：
2022-05-16
影响因子：
3.4
通讯作者：
Neaton, Jeffrey B.
中科院分区：
文献类型：
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作者：
Gant, Stephen E.;Haber, Jonah B.;Neaton, Jeffrey B.
在GW近似下的从头算多体微扰理论对用于计算准粒子修正的本征系统的依赖性限制了该方法的预测能力。在此，我们研究了最近开发的万尼尔局域化最优调谐屏蔽范围分离杂化（WOT - SRSH）泛函作为一系列半导体和绝缘体的单次GW（G(0)W(0)）计算的广义科恩 - 沈起始点的准确性。与基于成熟泛函（即PBE、PBE0和HSE）的计算以及与自洽GW方案和实验进行比较，结果表明通过G(0)W(0)@WOT - SRSH计算的带隙具有与更先进的方法（如准粒子自洽GW和本征值自洽GW）相当的精度和准确性水平。我们还发现G(0)W(0)@WOT - SRSH改进了对价带流形中更深能级状态的描述。最后，我们表明G(0)W(0)@WOT - SRSH显著降低了计算带隙对基础WOT - SRSH调谐过程中不确定性的敏感性。
The dependence of ab initio many-body perturbation theory within the GW approximation on the eigensystem used in calculating quasiparticle corrections limits this method's predictive power. Here, we investigate the accuracy of the recently developed Wannier-localized optimally tuned screened range-separated hybrid (WOT-SRSH) functional as a generalized Kohn-Sham starting point for single-shot GW (G(0)W(0)) calculations for a range of semiconductors and insulators. Comparison to calculations based on well-established functionals, namely, PBE, PBE0, and HSE, as well as to self-consistent GW schemes and to experiment, shows that band gaps computed via G(0)W(0)@WOT-SRSH have a level of precision and accuracy that is comparable to that of more advanced methods such as quasiparticle self-consistent GW and eigenvalue self-consistent GW. We also find that G(0)W(0)@WOT-SRSH improves the description of states deeper in the valence band manifold. Finally, we show that G(0)W(0)@WOT-SRSH significantly reduces the sensitivity of computed band gaps to ambiguities in the underlying WOT-SRSH tuning procedure.