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Unconventional Field-Induced Spin Gap in an S=1/2 Chiral Staggered Chain

J. Liu, S. Kittaka, R. D. Johnson, T. Lancaster, J. Singleton, T. Sakakibara, Y. Kohama, J. van Tol, A. Ardavan, B. H. Williams, S. J. Blundell, Z. E. Manson, J. L. Manson, and P. A. Goddard
Phys. Rev. Lett. 122, 057207 – Published 8 February 2019
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Abstract

We investigate the low-temperature magnetic properties of the molecule-based chiral spin chain [Cu(pym)(H2O)4]SiF6·H2O (pym=pyrimidine). Electron-spin resonance, magnetometry and heat capacity measurements reveal the presence of staggered g tensors, a rich low-temperature excitation spectrum, a staggered susceptibility, and a spin gap that opens on the application of a magnetic field. These phenomena are reminiscent of those previously observed in nonchiral staggered chains, which are explicable within the sine-Gordon quantum-field theory. In the present case, however, although the sine-Gordon model accounts well for the form of the temperature dependence of the heat capacity, the size of the gap and its measured linear field dependence do not fit with the sine-Gordon theory as it stands. We propose that the differences arise due to additional terms in the Hamiltonian resulting from the chiral structure of [Cu(pym)(H2O)4]SiF6·H2O, particularly a uniform Dzyaloshinskii-Moriya coupling and a fourfold periodic staggered field.

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  • Received 30 August 2018

DOI:https://doi.org/10.1103/PhysRevLett.122.057207

© 2019 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

J. Liu1, S. Kittaka2, R. D. Johnson1, T. Lancaster3, J. Singleton4, T. Sakakibara2, Y. Kohama2, J. van Tol5, A. Ardavan1, B. H. Williams1, S. J. Blundell1, Z. E. Manson6, J. L. Manson6,*, and P. A. Goddard7,†

  • 1Department of Physics, Clarendon Laboratory, University of Oxford, Parks Road, Oxford OX1 3PU, United Kingdom
  • 2Institute for Solid State Physics, University of Tokyo, Kashiwa, Chiba 277-8581, Japan
  • 3Centre for Materials Physics, Durham University, South Road, Durham DH1 3LE, United Kingdom
  • 4National High Magnetic Field Laboratory, Los Alamos National Laboratory, MS-E536, Los Alamos, New Mexico 87545, USA
  • 5National High Magnetic Field Laboratory, Florida State University, Tallahassee, Florida 32310, USA
  • 6Department of Chemistry and Biochemistry, Eastern Washington University, Cheney, Washington 99004, USA
  • 7Department of Physics, University of Warwick, Gibbet Hill Road, Coventry, CV4 7AL, United Kingdom

  • *jmanson@ewu.edu
  • p.goddard@warwick.ac.uk

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Issue

Vol. 122, Iss. 5 — 8 February 2019

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  • Figure 1
    Figure 1

    Chain structure of [Cu(pym)(H20)4]SiF6·H2O. H atoms and [SiF6]2 counterions are omitted for clarity. The unit cell houses four inequivalent Cu(II) ions. Staggered elongated CuO bonds (green) correspond to the local g axes. Inset: View along c axis depicting fourfold rotation of the local environment about the chain direction.

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  • Figure 2
    Figure 2

    (a) Room temperature ESR spectra at 240 GHz. A DM interaction and spin diffusion could contribute to linewidth anisotropy [14]. (b) Orientation dependence of Cu(II) g factor () and linewidth () at 300 K. The line is a fit to g(θ)=(gmin2cos2θ+gmax2sin2θ)1/2. (c),(d) ESR data with field c. (c) Temperature dependence of ESR spectra at 73 GHz. (d) Frequency versus field (H) plot showing ESR peaks observed at 1.9 K using the labeling scheme in (c). Solid lines are fits to f=AHα with α values shown. Dashed line is the paramagnetic resonance with g=2. (e) Inset: Representative χ vs T data with H=0.2T. Solid line is the model χ(T)=χ1D(T)+χs/T described in the text. Main panel: Angular variation of χs. The line is a fit to a cos2 dependence. (f) Temperature dependence of the magnetic contribution to heat capacity at different Hc. Lines are fits to a gapped model. Inset shows resulting field dependence of the gap (squares, size corresponds to largest y-axis error), a linear fit to the data (black line), the best fit to SG model (blue dotted line), and gap size predicted by SG model from experimental g2s value (solid blue line).

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  • Figure 3
    Figure 3

    Classical spin configurations for the unit cell of (a) Cu-benzoate and (b) [Cu(pym)(H2O)4]SiF6·H2O in applied field H0X axis. Z is the chain direction. Also shown are relative directions of the twofold and fourfold staggered fields (h2s, h4s and h4s), and uniform DM interaction (Du) allowed in [Cu(pym)(H2O)4]SiF6·H2O. The XZ canting in (b) would minimize coupling between the spins and h2s.

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