Modified band alignment method to obtain hybrid functional accuracy from standard DFT: Application to defects in highly mismatched III-V:Bi alloys
Modified band alignment method to obtain hybrid functional accuracy from standard DFT: Application to defects in highly mismatched III-V:Bi alloys
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DOI：
10.1103/physrevmaterials.5.124601
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发表时间：
2021-12
影响因子：
3.4
通讯作者：
M. Polak;R. Kudrawiec;R. Jacobs;I. Szlufarska;D. Morgan
中科院分区：
文献类型：
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作者：
M. Polak;R. Kudrawiec;R. Jacobs;I. Szlufarska;D. Morgan
本文为纯 111-V (111-V:Bi) 材料和含 Bi 111-V (111-V:Bi) 材料提供了准确的理论缺陷能量数据库，并基于对局部和半局部泛函所得结果的修正，研究了高通量缺陷计算的有效方法。在 -5 至 5 的电荷态下研究了点缺陷以及最近邻和次近邻对缺陷。通过显着更慢、保真度更高的混合 Heyd-Scuseria-Ernzerhof (HSE) 和显着更快、保真度更低的局域密度近似 (LDA) 计算，对 Ga-V:Bi 系统（GaP:Bi、GaAs:Bi 和 GaSb:Bi）进行了彻底研究。在这两种方法中，虚假静电相互作用均通过弗雷索尔特校正进行校正。结果根据可用的实验结果进行了验证，并用于评估先前的带对准校正的准确性。这里，提出了一种改进的频带对齐方法，以便更好地从 LDA 值预测 HSE 值。所提出的方法允许以 LDA 的计算成本预测缺陷能量，其值近似于 HSE 函数的值（此处研究的系统大约快 20 倍）。对 In-V:Bi 材料中选定的点缺陷进行测试后，修正后的 LDA 值的缺陷水平与 HSE 的平均绝对误差 (MAE) = 0.175 eV。该方法在 CdX（X=S、Se、Te）系统中的缺陷和杂质外部数据库上得到进一步验证，得出 MAE = 0.194 eV。这些测试证明校正足以进行定性和半定量预测，并且可能表明可转移到许多半导体系统而不会显着损失准确性。剩余的In-V:Bi缺陷和所有Al-V:Bi缺陷的性质是使用改进的能带对准方法来预测的。
This paper provides an accurate theoretical defect energy database for pure and Bi-containing 111-V (111-V:Bi) materials and investigates efficient methods for high-throughput defect calculations based on corrections of results obtained with local and semi-local functionals. Point defects as well as nearest-neighbor and second-nearest-neighbor pair defects were investigated in charge states ranging from -5 to 5. Ga-V:Bi systems (GaP:Bi, GaAs:Bi, and GaSb:Bi) were thoroughly investigated with significantly slower, higher fidelity hybrid Heyd-Scuseria-Ernzerhof (HSE) and significantly faster, lower fidelity local density approximation (LDA) calculations. In both approaches spurious electrostatic interactions were corrected with the Freysoldt correction. The results were verified against available experimental results and used to assess the accuracy of a previous band alignment correction. Here, a modified band alignment method is proposed in order to better predict the HSE values from the LDA ones. The proposed method allows prediction of defect energies with values that approximate those from the HSE functional at the computational cost of LDA (about 20x faster for the systems studied here). Tests of selected point defects in In-V :Bi materials resulted in corrected LDA values having a mean absolute error (MAE) = 0.175 eV for defect levels vs. HSE. The method was further verified on an external database of defects and impurities in CdX (X=S, Se, Te) systems, yielding a MAE = 0.194 eV. These tests demonstrate the correction to be sufficient for qualitative and semi-quantitative predictions, and may suggest transferability to many semiconductor systems without significant loss in accuracy. Properties of the remaining In-V :Bi defects and all Al-V :Bi defects were predicted with the use of the modified band alignment method.