论文标题
在密度功能理论中正确的电子密度和能级比对的局部轨道缩放校正校正计算
Self-consistent calculation of localized orbital scaling correction for correct electron densities and energy level alignment in density functional theory
论文作者
论文摘要
最近开发的局部轨道缩放校正（LOSC）方法显示了在常规密度函数近似（DFAS）中系统地和大小一致降低定位误差的能力。将LOSC应用于常规DFA（LOSC-DFAS），可以对相关特性的描述（包括带隙，总能量和光发射光谱）进行大大改进。但是，仍然存在问题和问题：将LOSC应用于DFAS的应用主要是通过自一致的领域（SCF）方式，而以SCF方式将LOSC应用于DFA的结果很少。原因是最初提出的SCF-LOSC计算方法使用了近似的Hamiltonian，并且在实践中很容易遇到收敛问题。在这项工作中，我们使用正确的哈密顿量开发了一种新的SCF方法，并实现可靠的SCF-LOSC计算。我们证明了SCF-LOSC新的SCF方法正确描述分子解离过程的电子密度，总能量和能级比对，而传统的DFA或LOSC-DFA具有SCF后计算的能力，显示出较大的错误。这项工作表明，SCF-LOSC的新SCF方法将是研究大型电子密度和能级对齐问题的问题的有前途的方法。
The recently developed localized orbital scaling correction (LOSC) method shows the ability to systematically and size-consistently reduce the delocalization error existing in conventional density functional approximations (DFAs). Applying LOSC to conventional DFAs (LOSC-DFAs) gives much improvement for the description of related properties, including band gaps, total energies and photoemission spectra. However, concern and issue remain: the application of LOSC to DFAs is mainly through a post self-consistent field (SCF) manner, and few results from applying LOSC to DFAs with a SCF manner have been reported. The reason is the originally proposed SCF approach for SCF-LOSC calculation uses an approximate Hamiltonian and encounters convergence problems easily in practice. In this work, we develop a new SCF approach with a correct Hamiltonian and achieve reliable SCF-LOSC calculations. We demonstrate the capability of the new SCF approach for SCF-LOSC to correctly describe the electron densities, total energies and energy level alignment for the molecular dissociation process, while conventional DFAs or LOSC-DFAs with post-SCF calculations show large errors. This work demonstrates that the new SCF approach for SCF-LOSC would be a promising method to study problems for correct electron densities and energy level alignment in large systems.
