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  Transient metal-centered states mediate isomerization of a photochromic ruthenium-sulfoxide complex

Cordones, A. A., Lee, J. H., Hong, K., Cho, H., Garg, K., Boggio-Pasqua, M., et al. (2018). Transient metal-centered states mediate isomerization of a photochromic ruthenium-sulfoxide complex. Nature Communications, 9: 1989. doi:10.1038/s41467-018-04351-0.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0002-4E56-7 Version Permalink: http://hdl.handle.net/21.11116/0000-0002-4E57-6
Genre: Journal Article

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This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article ’ s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article ’ s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.
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2018
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https://dx.doi.org/10.1038/s41467-018-04351-0 (Publisher version)
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 Creators:
Cordones, A. A.1, Author
Lee, J. H.2, Author
Hong, K.3, Author
Cho, H.4, Author
Garg, K.5, Author
Boggio-Pasqua, M.6, Author
Rack, J. J.5, 7, Author
Huse, N.8, 9, 10, Author              
Schoenlein, R. W.1, 11, Author
Kim, T. K.12, Author
Affiliations:
1PULSE Institute, SLAC National Accelerator Laboratory, Stanford University, ou_persistent22              
2Pohang Accelerator Laboratory, ou_persistent22              
3Center for Gas Analysis, Division of Chemical and Medical Metrology, Korea Research Institute of Standards and Science, ou_persistent22              
4Center for Analytical Chemistry, Division of Chemical and Medical Metrology, Korea Research Institute of Standards and Science, ou_persistent22              
5Nanoscale and Quantum Phenomena Institute, Department of Chemistry and Biochemistry, Ohio University, ou_persistent22              
6Laboratoire de Chimie et Physique Quantiques, CNRS et Université de Toulouse, ou_persistent22              
7Department of Chemistry & Chemical Biology, The University of New Mexico, ou_persistent22              
8Institute for Nanostructure and Solid State Physics, Department of Physics, University of Hamburg, ou_persistent22              
9Ultrafast Molecular Dynamics, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938289              
10Center for Free-Electron Laser Science, ou_persistent22              
11LCLS, SLAC National Accelerator Laboratory, ou_persistent22              
12Department of Chemistry and Chemistry Institute of Functional Materials, Pusan National University, ou_persistent22              

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 Abstract: Ultrafast isomerization reactions underpin many processes in (bio)chemical systems and molecular materials. Understanding the coupled evolution of atomic and molecular structure during isomerization is paramount for control and rational design in molecular science. Here we report transient X-ray absorption studies of the photo-induced linkage isomerization of a Ru-based photochromic molecule. X-ray spectra reveal the spin and valence charge of the Ru atom and provide experimental evidence that metal-centered excited states mediate isomerization. Complementary X-ray spectra of the functional ligand S atoms probe the nuclear structural rearrangements, highlighting the formation of two metal-centered states with different metal-ligand bonding. These results address an essential open question regarding the relative roles of transient charge-transfer and metal-centered states in mediating photoisomerization. Global temporal and spectral data analysis combined with time-dependent density functional theory reveals a complex mechanism for photoisomerization with atomic details of the transient molecular and electronic structure not accessible by other means.

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Language(s): eng - English
 Dates: 2017-07-262018-04-242018-05-18
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1038/s41467-018-04351-0
 Degree: -

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Project name : This work was supported by the U.S. Department of Energy, Of fi ce of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. This research used resources of the Advanced Light Source, Lawrence Berkeley National Laboratory, which is a DOE Of fi ce of Science User Facility. T.K.K. acknowledges funding from the National Research Foundation (NRF) grants, funded by the Ministry of Science and ICT (No. 2016K2A9A1A01945137, 2016R1E1A1A01941978, 2014R1A4A1001690, and 2016K1A4A4A01922028). N.H. acknowledges funding from the Max Planck Society, the City of Hamburg, and the German Science Foundation (DFG) through the SFB 925 “ Light induced dynamics and control of correlated quantum systems ” . J.J.R. and K.G. acknowledge funding from the National Science Foundation (CHE 0947031, CHE 1112250, and CHE 1602240).
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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
 Creator(s):
Affiliations:
Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 9 Sequence Number: 1989 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723