Efficient Semiclassical Evaluation of Electronic Coherences in Polyatomic Molecules.

Area of Science:

• Quantum dynamics
• Molecular physics
• Computational chemistry

Background:

• Light-induced processes in molecules lead to nonstationary quantum states.
• Simulating correlated electron-nuclear dynamics in polyatomic molecules is computationally challenging.

Purpose of the Study:

• To present a novel theoretical approach for simulating light-induced ultrafast dynamics in molecules.
• To couple electronic coherences with nuclear motion for accurate simulations.

Main Methods:

• Combines ab initio on-the-fly electronic structure calculations.
• Employs an efficient semiclassical procedure for nuclear wave packet dynamics.

Main Results:

• The method provides computationally efficient simulations of electronic coherences.
• It allows investigation of decoherence and revival phenomena driven by nuclear rearrangement.

Conclusions:

• The developed technique offers a powerful tool for understanding light-induced molecular dynamics.
• It facilitates insights into the physical mechanisms governing electronic coherences.