Ab initio lifetime correction to scattering states for time-dependent electronic-structure calculations with incomplete basis sets

作者：Coccia Emanuele; Assaraf Roland; Luppi Eleonora^*; Toulouse Julien

来源：Journal of Chemical Physics, 2017, 147(1): 014106.

DOI：10.1063/1.4991563

We propose a method for obtaining effective lifetimes of scattering electronic states for avoiding the artificial confinement of the wave function due to the use of incomplete basis sets in time-dependent electronic-structure calculations of atoms and molecules. In this method, using a fitting procedure, the lifetimes are extracted from the spatial asymptotic decay of the approximate scattering wave functions obtained with a given basis set. The method is based on a rigorous analysis of the complex-energy solutions of the Schrodinger equation. It gives lifetimes adapted to any given basis set without using any empirical parameters. The method can be considered as an ab initio version of the heuristic lifetime model of Klinkusch et al. [J. Chem. Phys. 131, 114304 (2009)]. The method is validated on H and He atoms using Gaussian-type basis sets for the calculation of high-harmonic-generation spectra. Published by AIP Publishing.

• 出版日期2017-7-7