ArticleThe journal of physical chemistry. A2026
Spatial Mapping of Valence Excited-State Landscapes Using Time-Resolved Shake-Down Spectroscopy.
Article in The journal of physical chemistry. A, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Time-resolved X-ray photoelectron spectroscopy (XPS) is used to track the photodissociation dynamics of 2-iodothiophene following 262 nm excitation. The transient XPS features include both direct ionization of the initially populated excited states and pronounced satellite peaks arising from shake-down processes. While the direct ionization signals exhibit only minimal energy shifts during C-I bond cleavage, the shake-down transitions undergo a substantial, 5 eV, shift over the reaction coordinate. By correlating these shifts with simulated C-I bond lengths, a direct structural mapping is established that reveals the exceptional sensitivity of shake-down channels to molecular geometry. These results demonstrate that shake-down transitions provide a new and powerful probe of ultrafast structural dynamics.
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