Light-Induced Radical Formation and Isomerization of an Aromatic Thiol in 
Solution Followed by Time-Resolved X-ray Absorption Spectroscopy at the Sulfur 
K-Edge

Ochmann, Miguel; von Ahnen, Inga; Cordones, Amy A.; Hussain, Abid; Lee, Jae Hyuk; Hong, Kiryong; Adamczyk, Katrin; Vendrell, Oriol; Kim, Tae Kyu; Schoenlein, Robert W.; Huse, Nils

doi:10.1021/jacs.6b12992

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Light-Induced Radical Formation and Isomerization of an Aromatic Thiol in Solution Followed by Time-Resolved X-ray Absorption Spectroscopy at the Sulfur K-Edge

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Ochmann, Miguel
International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Department of Physics, University of Hamburg and Center for Free Electron Laser Science, 22761 Hamburg, Germany;
Max Planck Institute for the Structure and Dynamics of Matter, 22761 Hamburg, Germany;

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Hussain, Abid
International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Department of Physics, University of Hamburg and Center for Free Electron Laser Science, 22761 Hamburg, Germany;
Max Planck Institute for the Structure and Dynamics of Matter, 22761 Hamburg, Germany;

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https://doi.org/10.1021/jacs.6b12992
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引用

Ochmann, M., von Ahnen, I., Cordones, A. A., Hussain, A., Lee, J. H., Hong, K., Adamczyk, K., Vendrell, O., Kim, T. K., Schoenlein, R. W., & Huse, N. (2017). Light-Induced Radical Formation and Isomerization of an Aromatic Thiol in Solution Followed by Time-Resolved X-ray Absorption Spectroscopy at the Sulfur K-Edge. Journal of the American Chemical Society, 139(13), 4797-4804. doi:10.1021/jacs.6b12992.

引用: https://hdl.handle.net/11858/00-001M-0000-002D-5496-5

要旨

We applied time-resolved sulfur-1s absorption
spectroscopy to a model aromatic thiol system as a promising method for tracking chemical reactions in solution. Sulfur-1s absorption spectroscopy allows tracking multiple sulfur species with a time resolution of ∼70 ps at synchrotron radiation facilities. Experimental transient spectra combined with high-level electronic structure theory allow identiﬁcation of a radical and two thione isomers, which are generated upon illumination with 267 nm radiation. Moreover, the regioselectivity of the
thione isomerization is explained by the resulting radical frontier orbitals. This work demonstrates the usefulness and potential of time-resolved sulfur-1s absorption spectroscopy for tracking multiple chemical reaction pathways and transient products of sulfur-containing molecules in solution.