Mapping rotational coherences onto time-resolved photoelectron imaging observables

Area of Science:

• Physical Chemistry
• Quantum Dynamics
• Spectroscopy

Background:

• Time-resolved photoelectron imaging is an advanced pump-probe spectroscopy technique.
• Its popularity is increasing due to its ability to probe ultrafast dynamics.
• Understanding the information content is crucial for its application.

Purpose of the Study:

• To explore the information content of time-resolved photoelectron imaging.
• To establish a theoretical and numerical framework for analyzing the technique's data.
• To connect wave packet properties to observable photoelectron image characteristics.

Main Methods:

• Theoretical modeling of time-evolving wave packets.
• Numerical simulations of photoelectron imaging experiments.
• Analysis of the relationship between wave packet alignment and image moments.

Main Results:

• A clear mapping between wave packet alignment properties and photoelectron image moments was identified.
• The origin and consequences of this mapping were investigated theoretically and numerically.
• The study quantifies the information obtainable from photoelectron images regarding electronic dynamics.

Conclusions:

• Time-resolved photoelectron imaging provides rich information about quantum dynamics.
• The established mapping enhances the interpretation of experimental data.
• This work advances the understanding and application of this powerful pump-probe technique.