论文标题
全电子周期性$ G_0W_0 $实现具有数值原子轨道基础功能:算法和基准测试
All-electron periodic $G_0W_0$ implementation with numerical atomic orbital basis functions: algorithm and benchmarks
论文作者
论文摘要
我们在数值原子轨道(NAO)基框架内提出了全电子定期{\ gnwn}。采用了确定性(RI)近似的局部变体,以显着降低评估和存储两电子库仑排斥积分的计算成本。我们证明,通过增强辅助基函数集的集合,用于扩展两个单粒子NAOS的产物,可以将局部RI近似产生的误差降低到微不足道的水平。引入了一种有效的算法来处理适合NAO框架的Brillouin区采样中的库仑奇异性。我们执行系统的收敛测试并确定一组计算参数,这些计算参数可以作为大多数实际目的的默认选择。对一组原型半导体和绝缘子进行了基准计算,并将基于线性性增强平面波(LAPW)以及高能局部轨道(HLOS)基于的独立$ G_0W_0 $实现获得的独立参考值进行了比较。使用中等(FHI-AIMS \ textIt {tier} 2)NAO基集,我们的$ G_0W_0 $计算产生的频段间隙通常位于标准LAPW和LAPW+HLO结果之间。与高度局部的Slater型轨道(STOS)补充\ textit {tier} 2,我们发现所获得的频带差距显示出对LAPW+HLO结果的总体收敛。在这项工作中开发的算法和技术为在NAO框架内有效实现相关方法的有效实现铺平了道路。
We present an all-electron, periodic {\GnWn} implementation within the numerical atomic orbital (NAO) basis framework. A localized variant of the resolution-of-the-identity (RI) approximation is employed to significantly reduce the computational cost of evaluating and storing the two-electron Coulomb repulsion integrals. We demonstrate that the error arising from localized RI approximation can be reduced to an insignificant level by enhancing the set of auxiliary basis functions, used to expand the products of two single-particle NAOs. An efficient algorithm is introduced to deal with the Coulomb singularity in the Brillouin zone sampling that is suitable for the NAO framework. We perform systematic convergence tests and identify a set of computational parameters, which can serve as the default choice for most practical purposes. Benchmark calculations are carried out for a set of prototypical semiconductors and insulators, and compared to independent reference values obtained from an independent $G_0W_0$ implementation based on linearized augmented plane waves (LAPW) plus high-energy localized orbitals (HLOs) basis set, as well as experimental results. With a moderate (FHI-aims \textit{tier} 2) NAO basis set, our $G_0W_0$ calculations produce band gaps that typically lie in between the standard LAPW and the LAPW+HLO results. Complementing \textit{tier} 2 with highly localized Slater-type orbitals (STOs), we find that the obtained band gaps show an overall convergence towards the LAPW+HLO results. The algorithms and techniques developed in this work pave the way for efficient implementations of correlated methods within the NAO framework.