周期固体中的非周期缺陷
Aperiodic defects in periodic solids
AI总结：
本文提出一种“无缺陷”嵌入方法，在原胞计算中构建嵌入场后引入单一非周期缺陷，避免周期性超胞带来的非物理伪影和慢收敛问题，并可结合后Hartree-Fock方法研究强关联缺陷与局域激发态。
摘要：
迄今为止，用于模拟缺陷（空位、吸附物等）的计算方法依赖于周期性超胞，其中缺陷与其重复镜像之间的距离足够远，以至于可以假设它们之间不存在相互作用。然而，缺陷镜像的相对邻近性和周期性重复可能会导致虚假的、非物理的伪影，尤其是当缺陷带电和/或为开壳层时，会导致向热力学极限（TDL）的收敛非常缓慢。在本快报中，我们引入了一种“无缺陷”嵌入形式，使得嵌入场在纯净的、原胞计算中求得。随后，在嵌入片段内部引入一个单一（即“非周期”）缺陷，该缺陷也可以带电。通过消除对补偿背景电荷和缺陷周期性的需要，我们规避了所有相关的非物理性和数值问题，实现了向热力学极限的极快收敛。此外，利用后Hartree-Fock方法的工具箱，该方案可以直接应用于研究强关联缺陷、局域激发态以及其他现有周期性协议无法提供满意描述的问题。
英文摘要：
To date, computational methods for modeling defects (vacancies, adsorbates, etc.) rely on periodic supercells in which the defect is far enough from its repeated image such that they can be assumed non-interacting. Yet, the relative proximity and periodic repetition of the defect's images may lead to spurious, unphysical artifacts, especially if the defect is charged and/or open-shell, causing a very slow convergence to the thermodynamic limit (TDL). In this Letter, we introduce a "defectless" embedding formalism such that the embedding field is computed in a pristine, primitive-unit-cell calculation. Subsequently, a single (i.e. "aperiodic") defect, which can also be charged, is introduced inside the embedded fragment. By eliminating the need for compensating background charges and periodicity of the defect, we circumvent all associated unphysicalities and numerical issues, achieving a very fast convergence to the TDL. Furthermore, using the toolbox of post-Hartree-Fock methods, this scheme can be straightforwardly applied to study strongly correlated defects, localized excited states and other problems, for which existing periodic protocols do not provide a satisfactory description.
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