The multielectron ionization dynamics underlying attosecond strong-field spectroscopies

Area of Science:

• Physical Chemistry
• Chemical Physics
• Quantum Dynamics

Background:

• Subcycle strong-field ionization (SFI) is crucial for attosecond electronic dynamics studies.
• Understanding multielectronic excitations in polyatomic molecules is essential for extending SFI methods.
• Theoretical models suggest multiple electronic continua participate in SFI of complex molecules.

Purpose of the Study:

• To experimentally probe the participation of multiple electronic continua in SFI dynamics of polyatomic molecules.
• To develop a theory-independent method for resolving SFI into distinct electronic-continuum channels.
• To advance spectroscopic techniques for studying attosecond electronic dynamics in complex molecules.

Main Methods:

• Utilized above-threshold ionization photoelectron spectroscopy.
• Employed photoelectron-photofragment coincidences.
• Investigated saturated (n-butane) and unsaturated (1,3-butadiene) linear hydrocarbons.

Main Results:

• Demonstrated direct experimental resolution of subcycle SFI into distinct electronic-continuum channels for polyatomic molecules.
• Showcased the applicability of the method to both saturated and unsaturated linear hydrocarbons.
• Provided experimental evidence for the direct participation of multiple electronic continua in SFI.

Conclusions:

• The developed method directly probes SFI dynamics in polyatomic molecules, independent of theoretical models.
• This technique is broadly applicable to various classes of polyatomic molecules.
• Advances the understanding of electron dynamics in complex molecular systems at the attosecond timescale.