Two-Dimensional Projected-Momentum Covariance Mapping for Coulomb Explosion Imaging

• Published in: The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Vol. 128; no. 16; pp. 3220 - 3229
• Main Authors: McManus, Joseph W., Allum, Felix, Featherstone, Josh, Lam, Chow-Shing, Brouard, Mark
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 25.04.2024
• Subjects: A: New Tools and Methods in Experiment and Theory; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
• ISSN: 1089-5639; 1520-5215
• DOI: 10.1021/acs.jpca.4c01084

We introduce projected-momentum covariance mapping, an extension of recoil-frame covariance mapping for 2D ion imaging studies. By considering the two-dimensional projection of the ion momenta as recorded by the detector, one opens the door to a complex suite of analysis tools adapted from three-dimensional momentum imaging studies. This includes the use of different frames of reference to unravel the dynamics of fragmentation and the application of fragment momentum constraints to isolate specific fragmentation channels. The technique is demonstrated on data from a two-dimensional ion imaging study of the Coulomb explosion of the cis and trans isomers of 1,2-dichloroethene, following strong-field ionization by an intense near-infrared femtosecond laser pulse. Classical simulations are used to guide the interpretation of projected-momentum covariance maps. The results offer a detailed insight into the distinct Coulomb explosion dynamics for this pair of isomers and lay the groundwork for future time-resolved studies of photoisomerization dynamics in this molecular system.