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Probing the electron motion in molecules using forward-scattering photoelectron holography
Optics Express
|January 4, 2024
Summary
Attosecond science now has a new way to observe charge migration in molecules. Forward-scattering photoelectron holography reveals shifts in electron patterns, accurately measuring electronic state dynamics.
Area of Science:
- Atomic, Molecular, and Optical Physics
- Quantum Dynamics
- Attosecond Science
Background:
- Charge migration, driven by electronic state superposition, is fundamental to intense laser-matter interactions.
- Observing ultrafast charge migration on its intrinsic attosecond timescale is a key challenge in modern physics.
- Current methods struggle to resolve the rapid dynamics of electronic wave packets in molecules.
Purpose of the Study:
- To theoretically demonstrate a novel scheme for probing molecular charge migration using forward-scattering photoelectron holography.
- To establish a method for observing charge migration on its natural attosecond timescale.
- To accurately determine the properties of superposition states, including relative phase and expansion coefficients.
Main Methods:
- Solving the time-dependent Schrödinger equation to obtain photoelectron momentum distributions (PEMDs).
- Utilizing strong-field tunneling ionization of molecules.
- Employing quantum-orbit analysis to interpret holographic interference patterns in PEMDs.
Main Results:
- A distinct shift in holographic interference patterns within PEMDs was observed for perpendicularly aligned molecules in a superposition state.
- This shift was directly linked to the time evolution of the non-stationary electronic superposition state.
- Accurate determination of the relative phase and expansion coefficient ratio of the involved electronic states was achieved by analyzing the momentum-dependent shift.
Conclusions:
- Forward-scattering photoelectron holography provides an efficient and accurate method for probing attosecond charge migration in molecules.
- The observed interference shift serves as a sensitive indicator of electronic wave packet dynamics.
- This technique holds promise for investigating electronic dynamics in increasingly complex molecular systems.
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