Tracking excited-state charge and spin dynamics in iron coordination complexes

Research output: Contribution to journalJournal article – Annual report year: 2014Researchpeer-review

  • Author: Zhang, Wenkai

    Stanford University, United States

  • Author: Alonso-Mori, Roberto

    SLAC National Accelerator Laboratory, United States

  • Author: Bergmann, Uwe

    SLAC National Accelerator Laboratory, United States

  • Author: Bressler, Christian

    European XFEL, Germany

  • Author: Chollet, Matthieu

    SLAC National Accelerator Laboratory, United States

  • Author: Galler, Andreas

    European XFEL

  • Author: Gawelda, Wojciech

    European XFEL

  • Author: Hadt, Ryan G.

    Stanford University, United States

  • Author: Hartsock, Robert W.

    Stanford University, United States

  • Author: Kroll, Thomas

    Stanford University, United States

  • Author: Kjær, Kasper Skov

    Neutrons and X-rays for Materials Physics, Department of Physics, Technical University of Denmark, Fysikvej, 2800, Kgs. Lyngby, Denmark

  • Author: Kubicek, Katharina

    Deutsches Elektronen-Synchrotron, Germany

  • Author: Lemke, Henrik Till

    SLAC National Accelerator Laboratory

  • Author: Liang, Huiyang W.

    Stanford University, United States

  • Author: Meyer, Drew A.

    Stanford University, United States

  • Author: Nielsen, Martin Meedom

    Neutrons and X-rays for Materials Physics, Department of Physics, Technical University of Denmark, Fysikvej, 2800, Kgs. Lyngby, Denmark

  • Author: Purser, Carola

    Stanford University, United States

  • Author: Robinson, Joseph S.

    SLAC National Accelerator Laboratory, United States

  • Author: Solomon, Edward I.

    SLAC National Accelerator Laboratory, United States

  • Author: Sun, Zheng

    Stanford University, United States

  • Author: Sokaras, Dimosthenis

    SLAC National Accelerator Laboratory, United States

  • Author: Brandt van Driel, Tim

    Neutrons and X-rays for Materials Physics, Department of Physics, Technical University of Denmark, Fysikvej, 2800, Kgs. Lyngby, Denmark

  • Author: Vankó, György

    Hungarian Academy of Sciences, Hungary

  • Author: Weng, Tsu-Chien

    SLAC National Accelerator Laboratory, United States

  • Author: Zhu, Diling

    SLAC National Accelerator Laboratory, United States

  • Author: Gaffney, Kelly J.

    Stanford University, United States

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Crucial to many light-driven processes in transition metal complexes is the absorption and dissipation of energy by 3d electrons(1-4). But a detailed understanding of such non-equilibrium excited-state dynamics and their interplay with structural changes is challenging: a multitude of excited states and possible transitions result in phenomena too complex to unravel when faced with the indirect sensitivity of optical spectroscopy to spin dynamics(5) and the flux limitations of ultrafast X-ray sources(6,7). Such a situation exists for archetypal poly-pyridyl iron complexes, such as [Fe(2,2'-bipyridine)(3)](2+), where the excited-state charge and spin dynamics involved in the transition from a low-to a high-spin state (spin crossover) have long been a source of interest and controversy(6-15). Here we demonstrate that femtosecond resolution X-ray fluorescence spectroscopy, with its sensitivity to spin state, can elucidate the spin crossover dynamics of [Fe(2,2'-bipyridine)(3)](2+) on photoinduced metal-to-ligand charge transfer excitation. We are able to track the charge and spin dynamics, and establish the critical role of intermediate spin states in the crossover mechanism. We anticipate that these capabilities will make our method a valuable tool for mapping in unprecedented detail the fundamental electronic excited-state dynamics that underpin many useful light-triggered molecular phenomena involving 3d transition metal complexes.
Original languageEnglish
JournalNature
Volume509
Issue number7500
Pages (from-to)345-+
Number of pages13
ISSN0028-0836
DOIs
Publication statusPublished - 2014
CitationsWeb of Science® Times Cited: No match on DOI

    Research areas

  • Multidisciplinary, Ray-absorption spectroscopy, Transition-metal-complexes, Free-electron laser, Emission spectroscopy, Crossover dynamics, Iron, Research
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