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Coulomb Explosion Imaging as a Tool to Distinguish Between Stereoisomers

Coulomb Explosion Imaging as a Tool to Distinguish Between Stereoisomers

Published on: August 18, 2017

Analyzing angular distributions for two-step dissociation mechanisms in velocity map imaging.

Daniel B Straus¹, Lynne M Butler, Bridget W Alligood

¹Department of Chemistry and the James Franck Institute, University of Chicago, Chicago, Illinois 60637, USA.

The Journal of Physical Chemistry. A

|March 8, 2013

Summary

This study presents a new algorithm for analyzing molecular dissociation using velocity map imaging. The method deciphers product velocity distributions from two-step dissociation processes, enabling detailed study of secondary dissociation events.

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Area of Science:

Physical Chemistry
Chemical Physics
Molecular Dynamics

Background:

Velocity map imaging (VMI) is increasingly utilized for studying photoinduced molecular dissociation.
Analyzing complex dissociation mechanisms, particularly two-step processes, presents analytical challenges.
Existing methods struggle to deconvolute product velocities from sequential dissociation events.

Purpose of the Study:

To introduce a novel algorithm for analyzing VMI data from two-step molecular dissociation.
To enable the study of the secondary dissociation step, often obscured in net product velocities.
To determine the velocity vector distribution of products from the secondary dissociation event.

Main Methods:

Development of a forward-convolution fitting algorithm.
Analysis of net speed, P(vnet), and angular, β(vnet), distributions of dissociation products.
Application to a two-step dissociation mechanism involving C-X bond cleavage and subsequent radical dissociation.

Main Results:

The algorithm successfully deconvolutes the velocity vectors from the secondary dissociation step.
It allows for the determination of the secondary speed distribution, P(v1,2°), and angular distribution, I(θ2°).
Enables detailed characterization of the dissociation dynamics of unstable intermediate radicals.

Conclusions:

The presented algorithm provides a powerful tool for detailed analysis of complex molecular dissociation.
It overcomes limitations in studying secondary dissociation events using VMI.
Facilitates a deeper understanding of molecular fragmentation dynamics.