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Revealing Hot and Long-Lived Metastable Spin States in the Photoinduced Switching of Solvated Metallogrid Complexes with Femtosecond Optical and X-ray Spectroscopies

Naumova, Maria A. (author)
German Electron Synchrotron (DESY)
Kalinko, Aleksandr (author)
German Electron Synchrotron (DESY),University of Paderborn
Wong, Joanne W.L. (author)
University of Göttingen
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Abdellah, Mohamed (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,South Valley University
Geng, Huifang (author)
ELI Attosecond Light Pulse Source (ELI-ALPS),ELI-HU Non-profit Ltd
Domenichini, Edoardo (author)
University of Strasbourg
Meng, Jie (author)
Technical University of Denmark
Gutierrez, Sol Alvarez (author)
Technical University of Denmark
Mante, Pierre Adrien (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Hong Kong Polytechnic University
Lin, Weihua (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
Zalden, Peter (author)
European XFEL GmbH
Galler, Andreas (author)
European XFEL GmbH
Lima, Frederico (author)
European XFEL GmbH
Kubicek, Katharina (author)
European XFEL GmbH
Biednov, Mykola (author)
European XFEL GmbH
Britz, Alexander (author)
European XFEL GmbH
Checchia, Stefano (author)
Lund University,Lunds universitet,MAX IV-laboratoriet,MAX IV Laboratory
Kabanova, Victoria (author)
European Synchrotron Radiation Facility
Wulff, Michael (author)
European Synchrotron Radiation Facility
Zimara, Jennifer (author)
Max Planck Institute for Biophysical Chemistry
Schwarzer, Dirk (author)
Max Planck Institute for Biophysical Chemistry
Demeshko, Serhiy (author)
University of Göttingen
Murzin, Vadim (author)
German Electron Synchrotron (DESY),University of Wuppertal
Gosztola, David (author)
Argonne National Laboratory
Jarenmark, Martin (author)
Lund University,Lunds universitet,Berggrundsgeologi,Geologiska institutionen,Naturvetenskapliga fakulteten,Lithosphere and Biosphere Science,Department of Geology,Faculty of Science
Zhang, Jianxin (author)
Tianjin Polytechnic University
Bauer, Matthias (author)
University of Paderborn
Lawson Daku, Max Latevi (author)
University of Geneva
Gawelda, Wojciech (author)
Adam Mickiewicz University in Poznań,European XFEL GmbH
Khakhulin, Dmitry (author)
European XFEL GmbH
Bressler, Christian (author)
European XFEL GmbH,University of Hamburg
Meyer, Franc (author)
University of Göttingen
Zheng, Kaibo (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Technical University of Denmark
Canton, Sophie E. (author)
German Electron Synchrotron (DESY),ELI-HU Non-profit Ltd,ELI Attosecond Light Pulse Source (ELI-ALPS)
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 (creator_code:org_t)
2020-02-18
2020
English 9 s.
In: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 11:6, s. 2133-2141
  • Journal article (peer-reviewed)
Abstract Subject headings
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  • An atomistic understanding of the photoinduced spin-state switching (PSS) within polynuclear systems of d4-d7 transition metal ion complexes is required for their rational integration into light-driven reactions of chemical and biological interest. However, in contrast to mononuclear systems, the multidimensional dynamics of the PSS in solvated molecular arrays have not yet been elucidated due to the expected complications associated with the connectivity between the metal centers and the strong interactions with the surroundings. In this work, the PSS in a solvated triiron(II) metallogrid complex is characterized using transient optical absorption and X-ray emission spectroscopies on the femtosecond time scale. The complementary measurements reveal the photoinduced creation of energy-rich (hot) and long-lived quintet states, whose dynamics differ critically from their mononuclear congeners. This finding opens major prospects for developing novel schemes in solution-phase spin chemistry that are driven by the dynamic PSS process in compact oligometallic arrays.

Subject headings

NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)
NATURVETENSKAP  -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
NATURAL SCIENCES  -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)

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