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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

Ochmann, M., von Ahnen, I., Cordones, A. A., Hussain, A., Lee, J. H., Hong, K., et al. (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.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0002-4FEA-F Version Permalink: http://hdl.handle.net/21.11116/0000-0002-4FEB-E
Genre: Journal Article

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jacs.6b12992.pdf (Publisher version), 949KB
 
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https://dx.doi.org/10.1021/jacs.6b12992 (Publisher version)
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 Creators:
Ochmann, M.1, 2, Author              
von Ahnen, I.1, Author
Cordones, A. A.3, Author
Hussain, A.1, 2, Author              
Lee, J. H.3, Author
Hong, K.3, 4, Author
Adamczyk, K.1, 2, Author              
Vendrell, O.5, Author
Kim, T. K.4, Author
Schoenlein, R. W.3, Author
Huse, N.1, 2, Author              
Affiliations:
1Department of Physics, University of Hamburg and Center for Free Electron Laser Science, ou_persistent22              
2Ultrafast Molecular Dynamics, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938289              
3Ultrafast X-ray Science Lab, Chemical Sciences Division, Lawrence Berkeley National Laboratory, ou_persistent22              
4Department of Chemistry and Chemistry Institute of Functional Materials, Pusan National University, ou_persistent22              
5Center for Free-Electron Laser Science, DESY and The Hamburg Centre for Ultrafast Imaging, ou_persistent22              

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 Abstract: 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.

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Language(s): eng - English
 Dates: 2016-12-222017-02-202017-02-20
 Publication Status: Published in print
 Pages: 8
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 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/jacs.6b12992
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Title: Journal of the American Chemical Society
  Other : J. Am. Chem. Soc.
  Abbreviation : JACS
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 139 (13) Sequence Number: - Start / End Page: 4797 - 4804 Identifier: ISSN: 0002-7863
CoNE: /journals/resource/954925376870