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

Area of Science:

• Quantum dynamics
• Attoscience
• Molecular physics

Background:

• Attoscience utilizes ultrashort laser pulses to study electron-nuclear motion.
• Modeling these dynamics requires advanced computational methods.
• Current methods face challenges in simulating complex molecular systems.

Purpose of the Study:

• Introduce the trajectory-guided eXternal Field Ab Initio Multiple Spawning (XFAIMS) method.
• Validate XFAIMS against established quantum dynamics simulations.
• Demonstrate XFAIMS's capability for polyatomic molecules.

Main Methods:

• Developed XFAIMS for on-the-fly simulation of laser-excited molecular dynamics.
• Applied XFAIMS to LiH molecule photoexcitation with atto- and femtosecond pulses.
• Investigated nuclear motion effects on sulfine (H2CSO) photoexcitation using XFAIMS.

Main Results:

• XFAIMS results closely agree with numerically exact quantum dynamics for LiH.
• Successfully modeled atto- and femtosecond laser pulse dynamics.
• Showcased XFAIMS's ability to handle polyatomic molecules like sulfine.

Conclusions:

• XFAIMS is a reliable method for simulating attoscience experiments.
• The method accurately captures correlated electron-nuclear motion.
• XFAIMS provides insights into molecular dynamics in complex systems.