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X-ray Transient Absorption and Picosecond IR Spectroscopy of Fulvalene(tetracarbonyl)diruthenium on Photoexcitation

Authors

  • Dr. Michael R. Harpham,

    1. Chemical Sciences and Engineering, Argonne National Laboratory, 9700 S Cass Avenue, Lemont IL 60439 (USA)
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  • Son C. Nguyen,

    1. Department of Chemistry, University of California at Berkeley, Berkeley, CA 94720-1460 (USA)
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  • Dr. Zongrui Hou,

    1. Department of Chemistry, University of California at Berkeley, Berkeley, CA 94720-1460 (USA)
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  • Prof. Dr. Jeffrey C. Grossman,

    1. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139 (USA)
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  • Prof. Dr. Charles B. Harris,

    Corresponding author
    1. Department of Chemistry, University of California at Berkeley, Berkeley, CA 94720-1460 (USA)
    • Department of Chemistry, University of California at Berkeley, Berkeley, CA 94720-1460 (USA)
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  • Michael W. Mara,

    1. Department of Chemistry, Northwestern University, Evanston, IL 60208 (USA)
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  • Dr. Andrew B. Stickrath,

    1. Chemical Sciences and Engineering, Argonne National Laboratory, 9700 S Cass Avenue, Lemont IL 60439 (USA)
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  • Prof. Dr. Yosuke Kanai,

    Corresponding author
    1. Department of Chemistry, University of North Carolina at Chapel Hill, Lawrence Livermore National Laboratory, Chapel Hill, NC 27599-3290 (USA)
    • Department of Chemistry, University of North Carolina at Chapel Hill, Lawrence Livermore National Laboratory, Chapel Hill, NC 27599-3290 (USA)
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  • Dr. Alexie M. Kolpak,

    1. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139 (USA)
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  • Dr. Donghwa Lee,

    1. Department of Chemistry, University of North Carolina at Chapel Hill, Lawrence Livermore National Laboratory, Chapel Hill, NC 27599-3290 (USA)
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  • Dr. Di-Jia Liu,

    1. Chemical Sciences and Engineering, Argonne National Laboratory, 9700 S Cass Avenue, Lemont IL 60439 (USA)
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  • Justin P. Lomont,

    1. Department of Chemistry, University of California at Berkeley, Berkeley, CA 94720-1460 (USA)
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  • Prof. Dr. Kasper Moth-Poulsen,

    1. Department of Chemical and Biological Engineering, Chalmers University of Technology, 41296 Gothenburg (Sweden)
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  • Dr. Nikolai Vinokurov,

    1. Department of Chemistry, University of California at Berkeley, Berkeley, CA 94720-1460 (USA)
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  • Prof. Dr. Lin X. Chen,

    Corresponding author
    1. Chemical Sciences and Engineering, Argonne National Laboratory, 9700 S Cass Avenue, Lemont IL 60439 (USA)
    2. Department of Chemistry, Northwestern University, Evanston, IL 60208 (USA)
    • Chemical Sciences and Engineering, Argonne National Laboratory, 9700 S Cass Avenue, Lemont IL 60439 (USA)
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  • Prof. Dr. K. Peter C. Vollhardt

    Corresponding author
    1. Department of Chemistry, University of California at Berkeley, Berkeley, CA 94720-1460 (USA)
    • Department of Chemistry, University of California at Berkeley, Berkeley, CA 94720-1460 (USA)
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  • M.R.H. carried out all of the X-ray transient absorption studies. S.C.N. is responsible for the picosecond IR investigation. This study was enabled by the Office of Science of the Department of Energy through the Laboratory Directed Research and Development Program at Argonne National Laboratory under contract number DE-AC02-05CH11231, by the Sustainable Products and Solutions Program at UC Berkeley, and by the NSF [grant numbers CHE-0907800 (K.P.C.V.) and CHE-0909632 (C.B.H.)]. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by the Argonne National Laboratory, was supported by the U.S. DOE under contract number DE-AC02-06CH11357. D.L. and Y.K. thank the National Energy Research Scientific Computing Center (Office of Science of the U.S. Department of Energy under contract number DE-AC02-05CH11231) for computational resources. We acknowledge access to the Molecular Graphics and Computation Facility at UC Berkeley (NSF, grant numbers CHE-0840505 and CHE-0233882). K.M.-P. is obliged to the Danish Research Council (grant number 09-66585/FNU) for financial support. J.P.L. is grateful to the NSF and the S.C.N. for a Vietnam International Education Development (VIED) graduate research fellowship. We are indebted to Prof. Michael W. George, University of Nottingham, for preliminary TRIR experiments.

Abstract

original image

Bei Photoanregung ertappt: Der Fulvalen-Diruthenium-Komplex auf der linken Bildseite fängt Licht ein, was zum Ru-Ru-Bindungsbruch führt und ein langlebiges Triplett-Diradikal in syn-Konfiguration ergibt. Thermische Aktivierung dieser Spezies ermöglicht einen Triplett-Singulett-Übergang hin zu einem Anti-Diradikal, der zu dem wärmespeichernden Isomer (rechte Seite) führt.

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