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Chemical tunnel-splitting-engineering in a dysprosium-based molecular nanomagnet

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      Abstract

      Total control over the electronic spin relaxation in molecular nanomagnets is the ultimate goal in the design of new molecules with evermore realizable applications in spin-based devices. For single-ion lanthanide systems, with strong spin–orbit coupling, the potential applications are linked to the energetic structure of the crystal field levels and quantum tunneling within the ground state. Structural engineering of the timescale of these tunneling events via appropriate design of crystal fields represents a fundamental challenge for the synthetic chemist, since tunnel splittings are expected to be suppressed by crystal field environments with sufficiently high-order symmetry. Here, we report the long missing study of the effect of a non-linear ( C 4) to pseudo-linear ( D 4d) change in crystal field symmetry in an otherwise chemically unaltered dysprosium complex. From a purely experimental study of crystal field levels and electronic spin dynamics at milliKelvin temperatures, we demonstrate the ensuing threefold reduction of the tunnel splitting.

      Abstract

      Suppression of quantum tunneling in molecular magnets is key for their magnetic behaviours to be exploitable. Here, the authors show that tuning the geometry of lanthanide single-ion magnets leads to a suppression of the quantum tunneling, finding a three-fold reduction of the tunnel splitting upon changing the crystal field symmetry.

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      Most cited references 60

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      Dispersion and Absorption in Dielectrics I. Alternating Current Characteristics

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        Magnetic bistability in a metal-ion cluster

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          Molecular spintronics using single-molecule magnets.

          A revolution in electronics is in view, with the contemporary evolution of the two novel disciplines of spintronics and molecular electronics. A fundamental link between these two fields can be established using molecular magnetic materials and, in particular, single-molecule magnets. Here, we review the first progress in the resulting field, molecular spintronics, which will enable the manipulation of spin and charges in electronic devices containing one or more molecules. We discuss the advantages over more conventional materials, and the potential applications in information storage and processing. We also outline current challenges in the field, and propose convenient schemes to overcome them.
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            Author and article information

            Affiliations
            [1 ]ISNI 0000 0001 0674 042X, GRID grid.5254.6, Department of Chemistry, , University of Copenhagen, ; 2100 Copenhagen, Denmark
            [2 ]ISNI 0000 0004 1936 9713, GRID grid.5719.a, Institut für Physikalische Chemie, , Universität Stuttgart, ; Pfaffenwaldring 55, 70569 Stuttgart, Germany
            [3 ]ISNI 0000 0001 0674 042X, GRID grid.5254.6, Niels Bohr Institute, , University of Copenhagen, ; 2100 Copenhagen, Denmark
            [4 ]ISNI 0000000121839049, GRID grid.5333.6, Laboratory for Quantum Magnetism, , École Polytechnique Fédérale Lausanne, ; 1015 Lausanne, Switzerland
            [5 ]Escola Universitària Salesiana de Sarrià (EUSS), Passeig Sant Joan Bosco 74, 08017 Barcelona, Spain
            [6 ]ISNI 0000000123222966, GRID grid.6936.a, Forschungsneutronenquelle Heinz Maier-Leibnitz FRM II, , Technische Universität München, ; 85748 Garching, Germany
            [7 ]ISNI 0000 0004 0647 2236, GRID grid.156520.5, Institute Laue–Langevin, ; BP 156, 38042 Grenoble Cedex 9, France
            [8 ]ISNI 0000 0001 0576 2336, GRID grid.466773.7, University of Zaragoza, , CSIC-Instituto de Cìencia de Materiales de Aragón (ICMA), ; Pedro Cerbuna 12, 50009 Zaragoza, Spain
            [9 ]ISNI 0000 0004 1936 7558, GRID grid.189504.1, Department of Chemistry, , Boston University, ; Boston, MA 02215 USA
            [10 ]ISNI 0000 0001 0674 042X, GRID grid.5254.6, Present Address: Department of Chemistry, , University of Copenhagen, ; 2100 Copenhagen, Denmark
            [11 ]ISNI 0000 0001 2181 8870, GRID grid.5170.3, Present Address: Department of Chemistry, , Technical University of Denmark, ; 2800 Lyngby, Denmark
            [12 ]ISNI 0000 0004 1936 9713, GRID grid.5719.a, Present Address: Institute of Aerospace Thermodynamics, , Universität Stuttgart, ; Pfaffenwaldring 31, 70569 Stuttgart, Germany
            [13 ]ISNI 0000 0004 1804 3922, GRID grid.418900.4, Present Address: Instituto de Catálisis y Petroleoquímica – CSIC, ; 28049 Madrid, Spain
            Contributors
            ORCID: http://orcid.org/0000-0001-5405-9022, mikkel.agerbaek@chem.ku.dk
            ORCID: http://orcid.org/0000-0003-1255-2868, bendix@kiku.dk
            Journal
            Nat Commun
            Nat Commun
            Nature Communications
            Nature Publishing Group UK (London )
            2041-1723
            29 March 2018
            29 March 2018
            2018
            : 9
            29599433
            5876375
            3706
            10.1038/s41467-018-03706-x
            © The Author(s) 2018

            Open Access 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. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

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