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Coexistence of magnetic order and persistent spin dynamics in a quantum kagome antiferromagnet with no intersite mixing

A. Zorko, M. Pregelj, M. Klanjšek, M. Gomilšek, Z. Jagličić, J. S. Lord, J. A. T. Verezhak, T. Shang, W. Sun, and J.-X. Mi
Phys. Rev. B 99, 214441 – Published 27 June 2019

Abstract

One of the key questions concerning frustrated lattices that has lately emerged is the role of disorder in inducing spin-liquid-like properties. In this context, the quantum kagome antiferromagnet YCu3(OH)6Cl3, which has been recently reported as the first geometrically perfect realization of the kagome lattice with negligible magnetic/nonmagnetic intersite mixing and a possible quantum-spin-liquid ground state, is of particular interest. However, contrary to previous conjectures, here we show clear evidence of bulk magnetic ordering in this compound below TN=15 K by combining bulk magnetization and heat capacity measurements, and local-probe muon spin relaxation measurements. The magnetic ordering in this material is rather unconventional in several respects. First, a crossover regime where the ordered state coexists with the paramagnetic state extends down to TN/3 and, second, the fluctuation crossover is shifted far below TN. Moreover, persistent spin dynamics that is observed at temperatures as low as T/TN=1/300 could be a sign of emergent excitations of correlated spin loops or, alternatively, a sign of fragmentation of each magnetic moment into an ordered and a fluctuating part.

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  • Received 3 April 2019
  • Revised 3 June 2019

DOI:https://doi.org/10.1103/PhysRevB.99.214441

©2019 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

A. Zorko1,*, M. Pregelj1, M. Klanjšek1, M. Gomilšek1,2, Z. Jagličić3,4, J. S. Lord5, J. A. T. Verezhak6, T. Shang7, W. Sun8, and J.-X. Mi8

  • 1Jožef Stefan Institute, Jamova c. 39, SI-1000 Ljubljana, Slovenia
  • 2Centre for Materials Physics, Durham University, South Road, Durham, DH1 3LE, United Kingdom
  • 3Faculty of Civil and Geodetic Engineering, University of Ljubljana, SI-1000 Ljubljana, Slovenia
  • 4Institute of Mathematics, Physics and Mechanics, SI-1000 Ljubljana, Slovenia
  • 5ISIS Pulsed Neutron and Muon Source, STFC Rutherford Appleton Laboratory, Didcot OX11 0QX, United Kingdom
  • 6Laboratory for Muon Spin Spectroscopy, Paul Scherrer Institute, CH-5232 Villigen PSI, Switzerland
  • 7Laboratory for Multiscale Materials Experiments, Paul Scherrer Institute, CH-5232 Villigen PSI, Switzerland
  • 8Fujian Provincial Key Laboratory of Advanced Materials, Department of Materials Science and Engineering, College of Materials, Xiamen University, Xiamen 361005, Fujian Province, People's Republic of China

  • *andrej.zorko@ijs.si

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Vol. 99, Iss. 21 — 1 June 2019

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Images

  • Figure 1
    Figure 1

    A perfect kagome lattice of Cu2+ spin-1/2 ions (orange spheres) trapped within O4Cl2 octahedra in YCu3(OH)6Cl3, as view along (a) the c crystallographic axis and (b) the b crystallographic axis. The nearest-neighbor exchange interaction (lines) is mediated by OH groups. Y3+,O2,H+, and Cl ions are denoted by gray, red, black, and green spheres, respectively.

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  • Figure 2
    Figure 2

    (a) DC magnetization of YCu3(OH)6Cl3 normalized by the applied magnetic field. The inset shows a broader temperature range up to 300 K and emphasizes the sudden increase of magnetization below TN=15 K. (b) The real part χ and the imaginary part χ (inset) of the AC susceptibility measured in an AC field of 0.6 mT and zero DC magnetic field. The arrows highlight the shift of the χ and χ maxima with increasing frequency. (c) The temperature dependence of the heat capacity of YCu3(OH)6Cl3. The vertical dashed lines in all panels highlight the ordering temperature TN=15 K.

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  • Figure 3
    Figure 3

    The decay of the muon polarization in YCu3(OH)6Cl3 at (a) T>TN and (b) T<TN in zero field (ZF) and in various applied longitudinal (LF) magnetic fields (symbols). The solid lines correspond to two-component fits (shown individually by dashed lines for the ZF datasets). The majority component μ1 corresponds to f=77(3)% of the signal, and the minority component μ2 to 23(3)%. In (a) the μ1 component exhibits oscillations due to static nuclear fields in a μ-OH complex, while the decay of the μ2 component is due to much smaller nuclear fields, yielding the standard Kubo-Toyabe function [the solid lines correspond to the model of Eq. (1)]. In (b) both components exhibit a damped cosine time dependence [the solid lines correspond to the model of Eq. (4)]. The dotted line highlights the 1/3 level.

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  • Figure 4
    Figure 4

    The magnitude of the internal fields and the decay rate of the corresponding oscillations (inset) for the two μSR components in ZF at T<TN. The lines are guides to the eye.

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  • Figure 5
    Figure 5

    The temperature dependence of the muon polarization decay in (a) a weak and (b) a strong longitudinal applied field (symbols) compared to the internal fields. The solid lines correspond to a two-component exponential model given by Eq. (5). The individual components are shown for the faster-relaxing datasets (8.7 K) by dashed lines.

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  • Figure 6
    Figure 6

    The temperature dependence of the paramagnetic fraction in YCu3(OH)6Cl3, as deduced from the 8-mT datasets (see text for details). The vertical line denotes the ordering temperature TN=15 K.

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  • Figure 7
    Figure 7

    The temperature dependence of the longitudinal muon spin relaxation rate for the two μSR components μi. The arrows indicate the ratio λL,2/λL,1. The vertical line denotes the ordering temperature TN=15 K.

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