Department of Physics, University of Helsinki, P.O. Box 64, FI-00014 University of Helsinki, Finland.
J Chem Phys. 2012 Sep 14;137(10):104105. doi: 10.1063/1.4749272.
In the current work we apply the completeness-optimization paradigm [P. Manninen and J. Vaara, J. Comput. Chem. 27, 434 (2006)] to investigate the basis set convergence of the moments of the ground-state electron momentum density at the self-consistent field level of theory. We present a black-box completeness-optimization algorithm that can be used to generate computationally efficient basis sets for computing any property at any level of theory. We show that the complete basis set (CBS) limit of the moments of the electron momentum density can be reached more cost effectively using completeness-optimized basis sets than using conventional, energy-optimized Gaussian basis sets. By using the established CBS limits, we generate a series of smaller basis sets which can be used to systematically approach the CBS and to perform calculations on larger, experimentally interesting systems.
在当前的工作中，我们应用完备性优化范式 [P. Manninen 和 J. Vaara, J. Comput. Chem. 27, 434 (2006)] 来研究在自洽场理论水平下，基组对基态电子动量密度矩的收敛性。我们提出了一种黑盒完备性优化算法，可用于生成计算任何性质的高效计算基组，无论理论水平如何。我们表明，使用完备性优化基组比使用传统的能量优化高斯基组，可以更经济有效地达到电子动量密度矩的完全基集（CBS）极限。通过使用已建立的 CBS 极限，我们生成了一系列更小的基组，可用于系统地逼近 CBS，并对更大的、实验上有趣的系统进行计算。
