AI 中文总结
本文在FHI-aims中实现了ACBN0伪杂化密度泛函，通过Löwdin正交化投影子提高稳定性，在金属氧化物和氮化物基准上降低带隙误差至HSE06精度，并展示其在低维体系OER过电位计算中的适用性。
AI 中文摘要
我们提出了一种在数值原子中心轨道基组中实现Agapito-Curtarolo-Buongiorno Nardelli（ACBN0）伪杂化密度泛函的公式和实现。该方法在全电子、全势电子结构软件包FHI-aims中实现。该实现使用Löwdin正交化投影子，这提高了所测试系统自洽ACBN0迭代的稳定性。对于包括金属氧化物和氮化物在内的基准材料集，采用完全局域极限（FLL）作为双重计数处理的ACBN0相对于Perdew-Burke-Ernzerhof（PBE）和强约束且适当范化的（SCAN）泛函降低了总带隙误差，达到了与Heyd-Scuseria-Ernzerhof泛函（HSE06）相当的精度。对于使用相同数值设置计算的六种块体过渡金属氧化物，一次HSE06迭代的代价大约是使用Petukhov混合的相应ACBN0@PBE迭代的13-33倍。通过计算β-NiOOH(001)表面上的吸附和析氧反应（OER）过电位，展示了局域基组实现对低维系统的适用性。在正则化SCAN（rSCAN）弛豫结构上，基于rSCAN的单点ACBN0（ACBN0@rSCAN）使用“tight”数值设置，将反应步能量与HSE06的平均绝对偏差降低，并使估计的过电位向HSE06和Perdew-Burke-Ernzerhof杂化（PBE0）参考结果移动。
英文摘要
We present a formulation and implementation of the Agapito-Curtarolo-Buongiorno Nardelli (ACBN0) pseudo-hybrid density functional in a numeric atom-centered orbital basis. The method is realized in the all-electron, full-potential electronic-structure package FHI-aims. The implementation uses a Löwdin-orthogonalized projector, which improved the stability of the self-consistent ACBN0 iterations for the tested systems. For a benchmark set of materials including metal oxides and nitrides, ACBN0 with the fully localized limit (FLL) as the double-counting treatment reduces the aggregate band gap errors relative to the Perdew-Burke-Ernzerhof (PBE) and strongly constrained and appropriately normed (SCAN) functionals, reaching an accuracy comparable to the Heyd-Scuseria-Ernzerhof functional (HSE06). For six bulk transition metal oxides calculated with the same numerical settings, an HSE06 iteration is approximately 13-33 times as expensive as the corresponding ACBN0@PBE iteration with Petukhov mixing. The applicability of the localized-basis implementation to low-dimensional systems is demonstrated by calculations of adsorption and the oxygen evolution reaction (OER) overpotential on a $β$-NiOOH(001) surface. On regularized SCAN (rSCAN) relaxed structures, single point ACBN0 based on rSCAN (ACBN0@rSCAN) with the ``tight'' numerical settings reduces the mean absolute deviation of the reaction-step energies from HSE06 and shifts the estimated overpotential toward the HSE06 and Perdew-Burke-Ernzerhof hybrid (PBE0) reference results.
Comments28 pages, 7 figures
