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Radical-lanthanide ferromagnetic interaction in a TbIII bis-phthalocyaninato complex

Dorsa Komijani, Alberto Ghirri, Claudio Bonizzoni, Svetlana Klyatskaya, Eufemio Moreno-Pineda, Mario Ruben, Alessandro Soncini, Marco Affronte, and Stephen Hill
Phys. Rev. Materials 2, 024405 – Published 23 February 2018
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Abstract

Recent studies have highlighted the importance of organic ligands in the field of molecular spintronics, via which delocalized electron-spin density can mediate magnetic coupling to otherwise localized 4f moments of lanthanide ions, which show tremendous potential for single-molecule device applications. To this end, high-field/high-frequency electron paramagnetic resonance (EPR) spectroscopy is employed to study a neutral terbium bis-phthalocyaninato metalorganic complex, [TbPc2]0, with the aim of understanding the magnetic interaction between the Ising-like moment of the lanthanide ion and the unpaired spin density on the coordinating organic radical ligand. The measurements were performed on a previously unknown [TbPc2]0 structural phase crystallizing in the Pnma space group. EPR measurements on powder samples of [TbPc2]0 reveal an anisotropic spectrum, which is attributed to the spin-12 radical coupled weakly to the EPR-silent TbIII ion. Extensive double-axis rotation studies on a single crystal reveal two independent spin-12 signals with differently oriented (albeit identical) uniaxial g-tensors, in complete agreement with x-ray structural studies that indicate two molecular orientations within the unit cell. The easy-axis nature of the radical EPR spectra thus reflects the coupling to the Ising-like TbIII moment. This is corroborated by studies of the isostructural [YPc2]0 analog (where Y is nonmagnetic yttrium), which gives a completely isotropic radical EPR signal. The experimental results for the terbium complex are well explained on the basis of an effective model that introduces a weak ferromagnetic Heisenberg coupling between an isotropic spin-12 and an anisotropic spin-orbital moment, J=6, that mimics the known, strong easy-axis TbPc2 crystal-field interaction.

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  • Received 27 December 2017

DOI:https://doi.org/10.1103/PhysRevMaterials.2.024405

©2018 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied PhysicsQuantum Information, Science & Technology

Authors & Affiliations

Dorsa Komijani1,2, Alberto Ghirri3, Claudio Bonizzoni3,4, Svetlana Klyatskaya5, Eufemio Moreno-Pineda5, Mario Ruben5, Alessandro Soncini6, Marco Affronte3,4,*, and Stephen Hill1,2,†

  • 1Department of Physics, Florida State University, Tallahassee, Florida 32306, USA
  • 2National High Magnetic Field Laboratory, Tallahassee, Florida 32310, USA
  • 3CNR-Instituto Nanoscienze, via G. Campi 213A, 41125 Modena, Italy
  • 4Dipartimento di Scienze Fisiche, Informatiche e Matematiche, Università di Modena e Reggio Emilia, via G. Campi 213A, 41125 Modena, Italy
  • 5Karlsruhe Institute of Technology (KIT), Institute of Nanotechnology, Eggenstein-Leopoldshafen, Germany
  • 6School of Chemistry, The University of Melbourne, 3010 Victoria, Australia

  • *marco.affronte@unimore.it
  • shill@magnet.fsu.edu

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Issue

Vol. 2, Iss. 2 — February 2018

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