Electronic structure and soft-X-ray-induced photoreduction studies of iron-based magnetic polyoxometalates of type {(M)M5}12FeIII30 (M = MoVI, WVI)
| Autor: | T. V. Kuznetsova, Manuel Prinz, Wanli Yang, Christian Taubitz, Paul J. Ziemann, Christine Derks, Jean-Paul Kappler, Loïc Joly, Manfred Neumann, Andrei Postnikov, Karsten Kuepper, Ulf Wiedwald |
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| Přispěvatelé: | Universität Ulm - Ulm University [Ulm, Allemagne], Osnabrück University, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Laboratoire de Chimie et Physique - Approche Multi-échelle des Milieux Complexes (LCP-A2MC), Université de Lorraine (UL), Advanced Light Source [LBNL Berkeley] (ALS), Lawrence Berkeley National Laboratory [Berkeley] (LBNL), M.N. Mikheev Institute of Metal Physics (IMP), Ural Branch of Russian Academy of Sciences (UB RAS), Faculty of Physics |
| Rok vydání: | 2013 |
| Předmět: |
Absorption spectroscopy
Dichroism Photochemistry Linking Ligand 02 engineering and technology Electronic structure 010402 general chemistry 01 natural sciences Absorption Inorganic Chemistry Nuclear magnetic resonance Molecule Spectroscopy Molecular magnets Magnetic structure Magnetic circular dichroism Chemistry Physik (inkl. Astronomie) 021001 nanoscience & nanotechnology 0104 chemical sciences Crystallography Exchange interactions [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci] Absorption (chemistry) 0210 nano-technology Giant clusters |
| Zdroj: | Dalton Transactions Dalton Transactions, Royal Society of Chemistry, 2013, 42 (22), pp.7924-7935. ⟨10.1039/c3dt32759k⟩ |
| ISSN: | 1477-9234 1477-9226 |
| DOI: | 10.1039/c3dt32759k |
| Popis: | International audience; Giant Keplerate-type molecules with a \Mo72Fe30\ core show a number of very interesting properties, making them particularly promising for various applications. So far, only limited data on the electronic structure of these molecules from X-ray spectra and electronic structure calculations have been available. Here we present a combined electronic and magnetic structure study of three Keplerate-type nanospheres-two with a \Mo72Fe30\ core and one with a \W72Fe30\ core by means of X-ray absorption spectroscopy, X-ray magnetic circular dichroism (XMCD), SQUID magnetometry, and complementary theoretical approaches. Furthermore, we present detailed studies of the Fe3+-to-Fe2+ photoreduction process, which is induced under soft X-ray radiation in these molecules. We observe that the photoreduction rate greatly depends on the ligand structure surrounding the Fe ions, with negatively charged ligands leading to a dramatically reduced photoreduction rate. This opens the possibility of tailoring such polyoxometalates by X-ray spectroscopic studies and also for potential applications in the field of X-ray induced photochemistry. |
| Databáze: | OpenAIRE |
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