Issue 25, 2023

Molecular photodissociation dynamics revealed by Coulomb explosion imaging


Coulomb explosion imaging (CEI) methods are finding ever-growing use as a means of exploring and distinguishing the static stereo-configurations of small quantum systems (molecules, clusters, etc). CEI experiments initiated by ultrafast (femtosecond-duration) laser pulses also allow opportunities to track the time-evolution of molecular structures, and thereby advance understanding of molecular fragmentation processes. This Perspective illustrates two emerging families of dynamical studies. ‘One-colour’ studies (employing strong field ionisation driven by intense near infrared or single X-ray or extreme ultraviolet laser pulses) afford routes to preparing multiply charged molecular cations and exploring how their fragmentation progresses from valence-dominated to Coulomb-dominated dynamics with increasing charge and how this evolution varies with molecular size and composition. ‘Two-colour’ studies use one ultrashort laser pulse to create electronically excited neutral molecules (or monocations), whose structural evolution is then probed as a function of pump–probe delay using an ultrafast ionisation pulse along with time and position-sensitive detection methods. This latter type of experiment has the potential to return new insights into not just molecular fragmentation processes but also charge transfer processes between moieties separating with much better defined stereochemical control than in contemporary ion-atom and ion-molecule charge transfer studies.

Graphical abstract: Molecular photodissociation dynamics revealed by Coulomb explosion imaging

Supplementary files

Article information

Article type
17 Apr 2023
01 Jun 2023
First published
02 Jun 2023
This article is Open Access
Creative Commons BY license

Phys. Chem. Chem. Phys., 2023,25, 16672-16698

Molecular photodissociation dynamics revealed by Coulomb explosion imaging

S. W. Crane, J. W. L. Lee, M. N. R. Ashfold and D. Rolles, Phys. Chem. Chem. Phys., 2023, 25, 16672 DOI: 10.1039/D3CP01740K

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