Department of Electrical and Computer Engineering, 100 Natural Resources Road, Marcus 201, University of Massachusetts, Amherst, Massachusetts 01003, USA.
J Chem Phys. 2013 May 21;138(19):194101. doi: 10.1063/1.4804419.
The self-consistent procedure in electronic structure calculations is revisited using a highly efficient and robust algorithm for solving the non-linear eigenvector problem, i.e., H({ψ})ψ = Eψ. This new scheme is derived from a generalization of the FEAST eigenvalue algorithm to account for the non-linearity of the Hamiltonian with the occupied eigenvectors. Using a series of numerical examples and the density functional theory-Kohn/Sham model, it will be shown that our approach can outperform the traditional SCF mixing-scheme techniques by providing a higher converge rate, convergence to the correct solution regardless of the choice of the initial guess, and a significant reduction of the eigenvalue solve time in simulations.
本文重新审视了电子结构计算中的自洽程序，使用一种高效、稳健的算法来求解非线性特征向量问题，即 H({ψ})ψ = Eψ。该新方案源自 FEAST 特征值算法的推广，以考虑占据特征向量的哈密顿量的非线性。通过一系列数值实例和密度泛函理论-Kohn/Sham 模型，我们的方法可以通过提供更高的收敛率、无论初始猜测如何都能收敛到正确的解以及在模拟中显著减少特征值求解时间，从而优于传统的 SCF 混合方案技术。
