Sheng Nan, Vorwerk Christian, Govoni Marco, Galli Giulia
Department of Chemistry, University of Chicago, Chicago, Illinois 60637, United States.
Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States.
J Chem Theory Comput. 2022 Jun 14;18(6):3512-3522. doi: 10.1021/acs.jctc.2c00240. Epub 2022 Jun 1.
We present a Green's function formulation of the quantum defect embedding theory (QDET) where a double counting scheme is rigorously derived within the approximation. We then show the robustness of our methodology by applying the theory with the newly derived scheme to several defects in diamond. Additionally, we discuss a strategy to obtain converged results as a function of the size and composition of the active space. Our results show that QDET is a promising approach to investigate strongly correlated states of defects in solids.
我们提出了量子缺陷嵌入理论（QDET）的格林函数公式，其中在近似范围内严格推导了一种双计数方案。然后，我们通过将该理论与新推导的方案应用于金刚石中的几种缺陷来展示我们方法的稳健性。此外，我们讨论了一种根据活性空间的大小和组成获得收敛结果的策略。我们的结果表明，QDET是研究固体中缺陷强关联态的一种有前途的方法。
