Predicting Coulomb explosion fragment angular distributions using molecular ground-state vibrational motion

Literature Information

Publication Date 2022-04-26
DOI 10.1039/D2CP01114J
Impact Factor 3.676
Authors

Louis Minion, Jason W. L. Lee, Michael Burt


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Abstract

Laser-induced Coulomb explosions can be used to identify gas-phase molecular structures through correlations between fragment ion trajectories. This report presents a model for predicting these outcomes, which first establishes the neutral equilibrium geometry of a target molecule using electronic structure calculations, and then samples a probability distribution of potential ground-state configurations by allowing for zero-point vibrational motion. Candidate structures are assumed to explode instantaneously into charged fragments, and the simulated ion trajectories are correlated using recoil-frame covariance analysis. The effects of detection efficiency and fluctuating experimental conditions are also considered. The results were found to match experimental data, indicating that Coulomb explosion fragment angular distributions produced from highly-charged ions depend largely on the internal motion of the target molecule.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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