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Free, publicly-accessible full text available July 1, 2024
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Chang, Kristina F. ; Reduzzi, Maurizio ; Wang, Han ; Poullain, Sonia M. ; Kobayashi, Yuki ; Barreau, Lou ; Prendergast, David ; Neumark, Daniel M. ; Leone, Stephen R. ( , Nature Communications)
Abstract Conical intersections between electronic states often dictate the chemistry of photoexcited molecules. Recently developed sources of ultrashort extreme ultraviolet (XUV) pulses tuned to element-specific transitions in molecules allow for the unambiguous detection of electronic state-switching at a conical intersection. Here, the fragmentation of photoexcited
iso- propyl iodide andtert- butyl iodide molecules (i -C3H7I andt -C4H9I) through a conical intersection between3Q0/1Q1spin–orbit states is revealed by ultrafast XUV transient absorption measuring iodine 4d core-to-valence transitions. The electronic state-sensitivity of the technique allows for a complete mapping of molecular dissociation from photoexcitation to photoproducts. In both molecules, the sub-100 fs transfer of a photoexcited wave packet from the3Q0state into the1Q1state at the conical intersection is captured. The results show how differences in the electronic state-switching of the wave packet ini -C3H7I andt -C4H9I directly lead to differences in the photoproduct branching ratio of the two systems. -
Barreau, Lou ; Petersson, C. Leon M. ; Klinker, Markus ; Camper, Antoine ; Marante, Carlos ; Gorman, Timothy ; Kiesewetter, Dietrich ; Argenti, Luca ; Agostini, Pierre ; González-Vázquez, Jesús ; et al ( , Physical Review Letters)