On the formation of anions: frequency-, angle-, and time-resolved photoelectron imaging of the menadione radical anion† †Electronic supplementary information (ESI) available: A summary of the ground-state geometries and molecular orbitals from the ab initio calculations; fitted residuals from the FA-PI simulation; plots of all spectra included in the frequency-resolved two-dimensional figure; and example time-resolved PE spectra from the 3.10 + 1.55 eV pump-probe experiments. See DOI: 10.1039/c4sc03491k Click here for additional data file.
نویسندگان
چکیده
Frequency-, angle-, and time-resolved photoelectron imaging of gas-phase menadione (vitamin K3) radical anions was used to show that quasi-bound resonances of the anion can act as efficient doorway states to produce metastable ground electronic state anions on a sub-picosecond timescale. Several anion resonances have been experimentally observed and identified with the assistance of ab initio calculations, and ground state anion recovery was observed across the first 3 eV above threshold. Timeresolved measurements revealed the mechanism of electronic ground state anion formation, which first involves a cascade of very fast internal conversion processes to a bound electronic state that, in turn, decays by slower internal conversion to the ground state. Autodetachment processes from populated resonances are inefficient compared with electronic relaxation through internal conversion. The mechanistic understanding gained provides insight into the formation of radical anions in biological and astrochemical systems.
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Resonances of the anthracenyl anion probed by frequency-resolved photoelectron imaging of collision-induced dissociated anthracene carboxylic acid† †Electronic supplementary information (ESI) available: Raw photoelectron spectra and images; fragment photoelectron spectra from 9- and 1-C14H9–CO2 – precursors; and excited state molecular orbital contributions. See DOI: 10.1039/c6sc05405f Click here for additional data file.
Resonances in polyaromatic hydrocarbon (PAH) anions are key intermediates in a number of processes such as electron transfer in organic electronics and electron attachment in the interstellar medium. Here we present a frequencyand angle-resolved photoelectron imaging study of the 9-anthracenyl anion generated through collision induced dissociation (CID) of its electrosprayed deprotonated anthra...
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Institut für Anorganische Chemie, Julius Hubland, 97074 Würzburg, Germany. E-ma School of Medicine, Pharmacy and Health, Stockton-on-Tees, TS17 6BH, UK Department of Chemistry, University of Tor M5S 3H6, Canada Institut für Organische Chemie, JuliusHubland, 97074 Würzburg, Germany † Electronic supplementary information Additional views of the molecular stru voltammograms of 2 and 3. Plots of ca...
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Department of Chemistry, University of Wa [email protected]; P.R.Unwin@warw School of Chemistry, Australian Resear Electromaterials Science, Monash University Department of Physics, University of Warwi † Electronic supplementary information ( resolved LSV-SECCM movies obtained f surface of bulk MoS2. Fig. S1 to S14 characterization of MoS2; SEM images of LSVs and Tafel plots obtained from...
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