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Chemistry. 2016 Jan 26;22(5):1779-88. doi: 10.1002/chem.201503431. Epub 2016 Jan 08.

Studies of a Large Odd-Numbered Odd-Electron Metal Ring: Inelastic Neutron Scattering and Muon Spin Relaxation Spectroscopy of Cr8 Mn.

Chemistry (Weinheim an der Bergstrasse, Germany)

Michael L Baker, Tom Lancaster, Alessandro Chiesa, Giuseppe Amoretti, Peter J Baker, Claire Barker, Stephen J Blundell, Stefano Carretta, David Collison, Hans U Güdel, Tatiana Guidi, Eric J L McInnes, Johannes S Möller, Hannu Mutka, Jacques Ollivier, Francis L Pratt, Paolo Santini, Floriana Tuna, Philip L W Tregenna-Piggott, Iñigo J Vitorica-Yrezabal, Grigore A Timco, Richard E P Winpenny

Affiliations

  1. School of Chemistry and Photon Science Institute, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK. [email protected].
  2. Institut Laue-Langevin, BP 156, 6?rue Jules Horowitz, 38042, Grenoble Cedex?9, France. [email protected].
  3. Department of Physics, Durham University, South Road, Durham, DH1 3LE, UK.
  4. Dipartimento di Fisica e Scienze della Terra, Università di Parma, 43124, Parma, Italy.
  5. ISIS Facility, Rutherford Appleton Laboratory, Didcot, OX11 0QX, UK.
  6. School of Chemistry and Photon Science Institute, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK.
  7. Clarendon Laboratory, Department of Physics, University of Oxford, OX1 3PU, UK. [email protected].
  8. Department of Chemistry and Biochemistry, University of Bern, 3000, Bern, Switzerland.
  9. Clarendon Laboratory, Department of Physics, University of Oxford, OX1 3PU, UK.
  10. Institut Laue-Langevin, BP 156, 6?rue Jules Horowitz, 38042, Grenoble Cedex?9, France.
  11. School of Chemistry and Photon Science Institute, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK. [email protected].

PMID: 26748964 PMCID: PMC4744977 DOI: 10.1002/chem.201503431

Abstract

The spin dynamics of Cr8 Mn, a nine-membered antiferromagnetic (AF) molecular nanomagnet, are investigated. Cr8 Mn is a rare example of a large odd-membered AF ring, and has an odd-number of 3d-electrons present. Odd-membered AF rings are unusual and of interest due to the presence of competing exchange interactions that result in frustrated-spin ground states. The chemical synthesis and structures of two Cr8 Mn variants that differ only in their crystal packing are reported. Evidence of spin frustration is investigated by inelastic neutron scattering (INS) and muon spin relaxation spectroscopy (μSR). From INS studies we accurately determine an appropriate microscopic spin Hamiltonian and we show that μSR is sensitive to the ground-spin-state crossing from S=1/2 to S=3/2 in Cr8 Mn. The estimated width of the muon asymmetry resonance is consistent with the presence of an avoided crossing. The investigation of the internal spin structure of the ground state, through the analysis of spin-pair correlations and scalar-spin chirality, shows a non-collinear spin structure that fluctuates between non-planar states of opposite chiralities.

© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Keywords: inelastic neutron scattering; molecular magnetism; muon spin relaxation; spin chirality; spin frustration

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