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Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation.

Jyoti Rajput¹, T Severt¹, Ben Berry¹

¹J. R. Macdonald Laboratory, Physics Department, Kansas State University, Manhattan, Kansas 66506, USA.

Physical Review Letters

|March 24, 2018

Summary

We developed a new method to distinguish sequential and concerted molecular fragmentation. This technique analyzes molecular breakup in its own frame, separating different dissociation pathways for polyatomic molecules.

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Area of Science:

Chemical Physics
Molecular Dynamics
Quantum Chemistry

Background:

Distinguishing between sequential and concerted dissociation mechanisms in polyatomic molecules is a fundamental challenge.
Understanding these fragmentation pathways is crucial for controlling molecular reactions and interpreting experimental data.

Purpose of the Study:

To develop and demonstrate a novel method for clearly separating sequential and concerted three-body fragmentation mechanisms.
To apply this method to laser-driven fragmentation of OCS and determine branching ratios.

Main Methods:

Utilized laser-driven fragmentation of OCS (carbonyl sulfide) molecules.
Employed coincidence momentum imaging to track fragment ions (O+, C+, S+).
Developed a novel native-frame analysis technique to separate dissociation events based on intermediate fragment rotation.

Main Results:

Successfully separated sequential and concerted breakup pathways for OCS fragmentation.
Determined the branching ratios for different fragmentation processes of OCS³⁺.
Observed that the first step of sequential breakup is aligned with laser polarization.
Identified electronic states of intermediate dications involved in dissociation.
Found preferential perpendicular ejection of the central carbon atom in concerted breakup relative to the laser field.

Conclusions:

The native-frame analysis method provides a clear distinction between sequential and concerted molecular fragmentation.
This method is versatile and applicable to various projectiles and molecular systems.
Detailed insights into the dynamics of each dissociation step and the electronic states involved were obtained.