Simplicity beneath Complexity: Counting Molecular Electrons Reveals Transients and Kinetics of Photodissociation Reactions

Jennifer M Ruddock, Nikola Zotev, Brian Stankus, Haiwang Yong, Darren Bellshaw, Sebastien Boutet, Thomas J Lane, Mengning Liang, Sergio Carbajo, Wenpeng Du, Adam Kirrander, Michael P Minitti, Peter M Weber

Research output: Contribution to journalArticlepeer-review

Abstract / Description of output

Time-resolved pump-probe gas phase X-ray scattering signals, extrapolated to zero momentum transfer, provide a measure of the number of electrons in a system, an effect that arises from the coherent addition of elastic scattering from the electrons. This allows for the identification of reactive transients and the determination of the chemical reaction kinetics without the need for extensive scattering simulations or complicated inversion of scattering data. We examine the photodissociation reaction of trimethyl amine, and identify two reaction paths upon excitation to the 3p state at 200 nm: a fast dissociation path out of the 3p state to the dimethyl amine radical (16.6±1.2%), and a slower dissociation via internal conversion to the 3s state (83.4±1.2%). The time constants for the two reactions are 640±130 fs and 74±6 ps, respectively. In addition, it is found that the transient dimethyl amine radical has a N-C bond length of 1.45±0.02 Å and a CNC bond angle of 118°±4
Original languageEnglish
JournalAngewandte Chemie International Edition
Early online date13 Mar 2019
DOIs
Publication statusE-pub ahead of print - 13 Mar 2019

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