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Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet αRuCl3

G. Bastien, G. Garbarino, R. Yadav, F. J. Martinez-Casado, R. Beltrán Rodríguez, Q. Stahl, M. Kusch, S. P. Limandri, R. Ray, P. Lampen-Kelley, D. G. Mandrus, S. E. Nagler, M. Roslova, A. Isaeva, T. Doert, L. Hozoi, A. U. B. Wolter, B. Büchner, J. Geck, and J. van den Brink
Phys. Rev. B 97, 241108(R) – Published 15 June 2018
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Abstract

Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material αRuCl3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin-liquid phase in αRuCl3 strongly competes with the crystallization of spin singlets into a valence bond solid.

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  • Received 26 January 2018

DOI:https://doi.org/10.1103/PhysRevB.97.241108

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

G. Bastien1,*, G. Garbarino2, R. Yadav1, F. J. Martinez-Casado3,4, R. Beltrán Rodríguez1, Q. Stahl5, M. Kusch5, S. P. Limandri6, R. Ray1,7, P. Lampen-Kelley8,9, D. G. Mandrus8,9, S. E. Nagler10, M. Roslova11, A. Isaeva11, T. Doert11, L. Hozoi1, A. U. B. Wolter1, B. Büchner1,5, J. Geck5, and J. van den Brink1,12,13

  • 1Leibniz-Institut für Festkörper- und Werkstoffforschung (IFW) Dresden, 01171 Dresden, Germany
  • 2European Synchrotron Radiation Facility, 38043 Grenoble, France
  • 3Institut Laue-Langevin, 38042 Grenoble, France
  • 4Instituto de Ciencia de Materiales de Aragón (ICMA), CSIC and Universidad de Zaragoza, 50009 Zaragoza, Spain
  • 5Institut für Festkörper- und Materialphysik, Technische Universität Dresden, 01062 Dresden, Germany
  • 6IFEG, CONICET, Medina Allende s/n, Ciudad Universitaria, 5000 Cordoba, Argentina
  • 7Dresden Center for Computational Materials Science (DCMS), Technische Universität Dresden, 01062 Dresden, Germany
  • 8Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 9Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, USA
  • 10Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 11Fakultät für Chemie und Lebensmittelchemie, Technische Universität Dresden, 01062 Dresden, Germany
  • 12Institut für Theoretische Physik, Technische Universität Dresden, 01062 Dresden, Germany
  • 13Department of Physics, Harvard University, Cambridge, Massachusetts 02138, USA

  • *g.bastien@ifw-dresden.de

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Vol. 97, Iss. 24 — 15 June 2018

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