Communication: XFAIMS—eXternal Field Ab Initio Multiple Spawning for electron-nuclear dynamics triggered by short laser pulses

Mignolet, Benoit; Curchod, Basile F.E.; Martínez, Todd J.

Abstract

Attoscience is an emerging field where attosecond pulses or few cycle IR pulses are used to pump and probe the correlated electron-nuclear motion of molecules. We present the trajectory-guided eXternal Field Ab Initio Multiple Spawning (XFAIMS) method that models such experiments “on-the-fly,” from laser pulse excitation to fragmentation or nonadiabatic relaxation to the ground electronic state. For the photoexcitation of the LiH molecule, we show that XFAIMS gives results in close agreement with numerically exact quantum dynamics simulations, both for atto- and femtosecond laser pulses. We then show the ability of XFAIMS to model the dynamics in polyatomic molecules by studying the effect of nuclear motion on the photoexcitation of a sulfine (H2CSO).

Citation

Mignolet, B., Curchod, B. F., & Martínez, T. J. (2016). Communication: XFAIMS—eXternal Field Ab Initio Multiple Spawning for electron-nuclear dynamics triggered by short laser pulses. The Journal of Chemical Physics, 145(19), Article 191104. https://doi.org/10.1063/1.4967761

• Journal Article Type: Article
• Acceptance Date: Nov 1, 2016
• Online Publication Date: Nov 16, 2016
• Publication Date: Nov 16, 2016
• Deposit Date: Nov 6, 2017
• Publicly Available Date: Dec 8, 2017
• Journal: Journal of Chemical Physics
• Print ISSN: 0021-9606
• Electronic ISSN: 1089-7690
• Publisher: American Institute of Physics
• Peer Reviewed: Peer Reviewed
• Volume: 145
• Issue: 19
• Article Number: 191104
• DOI: https://doi.org/10.1063/1.4967761
• Public URL: https://durham-repository.worktribe.com/output/1372177