Molecular Auger Interferometry

Area of Science:

• Molecular Physics
• Quantum Chemistry
• Spectroscopy

Background:

• Auger decay is a fundamental process in molecular physics.
• Measuring Auger decay lifetimes in molecules is crucial for understanding electron dynamics.
• Current methods often require high-resolution or attosecond spectroscopy.

Purpose of the Study:

• To introduce a novel theory for interferometric measurement of molecular Auger decay lifetimes.
• To demonstrate a method for extracting Auger lifetimes without advanced spectroscopic techniques.
• To validate the theory using inner-valence decay in methyl fluoride (CH3F).

Main Methods:

• Developing a theory of molecular Auger interferometry.
• Utilizing a two-color (ω/2ω) laser field for coherent phase control of Auger dynamics.
• Analyzing the modulation of total ionization yield by the relative phase in oriented molecules.

Main Results:

• The relative phase in a two-color laser field modulates the total ionization yield in oriented molecules.
• A simple analytical formula was derived to extract Auger lifetimes from interferograms.
• The principle was successfully demonstrated using inner-valence decay in CH3F.

Conclusions:

• Molecular Auger interferometry provides a new pathway for determining Auger decay lifetimes.
• This method circumvents the need for high-resolution or attosecond spectroscopy.
• The technique offers a simpler approach to studying ultrafast electron dynamics in molecules.