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

Mikkel Sorensen, Ursula Hansen, Mauro Perfetti, Kasper Pedersen, Elena Bartolome, Giovanna Simeoni, Hannu Mutka, Stephane Rols, Minki Jeong, Ivica Zivkovic, Maria Retuerto, Ana Arauzo, Juan Bartolome, Stergios Piligkos, Hogni Weihe, Linda Doerrer, Joris van Slageren, Henrik Ronnow, Kim Lefmann, Jesper Bendix

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35 Citations (Scopus)
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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 (C4) to pseudo-linear (D4d) 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.
Original languageEnglish
Article number1292
JournalNature Communications
Publication statusPublished - 29 Mar 2018


  • Coordination chemistry
  • Inorganic chemistry
  • Magnetic materials


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