[25a-D316-1~10] 3.6 Ultrashort-pulse and high-intensity lasers

▲ [25a-D316-10] Implementation of the time-dependent multiconfiguration method for diatomic molecules

〇(P)Yang Li¹, Takeshi Sato¹, Kenichi Ishikawa¹ (1.The Univ. of Tokyo)

Keywords:ultrafast phenomena, strong field ionization and dissociation, high harmonic generation

Multielectron dynamics plays an important role when atoms and molecules are subject to ultrashort intense laser pulses. Numerical investigations of multielectron dynamics and correlation effects require highly nonperturbative treatments, which are very challenging. In order to tackle this challenge, the time-dependent multiconfiguration self-consistent-field (TD-MCSCF) methods have been developed. In this contribution, we report two real-space implementations of the TD-CASSCF method for diatomic molecules. The first one focuses on the multielectron dynamics within the Born-Oppenheimer approximation. This implementation adopts prolate spheroidal coordinates with spatial grids discretized by a finite-element discrete variable representation, which offers an accurate representation of electron-nucleus interaction and high sparsity of the Hamiltonian operators. In the second implementation, we adopt the fully general TD-MCSCF method, in which protons and electrons are treated on an equal footing, to address the joint electron-nuclear dynamics in a strong laser field.