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Cluster glass transition and relaxation in the random spinel CoGa2O4

T. Naka, T. Nakane, S. Ishii, M. Nakayama, A. Ohmura, F. Ishikawa, A. de Visser, H. Abe, and T. Uchikoshi
Phys. Rev. B 103, 224408 – Published 4 June 2021

Abstract

We report magnetic properties in the random spinel magnet CoGa2O4. Rietveld analysis of the x-ray diffraction profile for CoGa2O4 reveals that the Co and Ga ions are distributed randomly in the tetrahedral A sites and octahedral B sites in the cubic spinel structure. CoGa2O4 exhibits a spin-glass transition at TSG=8.2K that is confirmed by measurements of the dc and ac susceptibilities and thermoremanent magnetization (TRM) that develops below TSG. From the frequency dependence of the freezing temperature Tf for CoGa2O4, it is indicated that the relaxation time τ(T) follows a Vogel-Fulcher law τ=τ0exp[Ea/kB(TT0)]. An analysis of specific heat suggested that a doublet ground state of the octahedrally coordinated Co2+ was stabilized by spin-orbit and crystal field couplings. The relaxation rate of TRM is considerably enhanced at TSG and decays rapidly above and below TSG. The time course of TRM is reproduced by nonexponential relaxation forms, such as a stretched exponential (Kohlrausch) as well as Ogielski and Weron relaxation forms. This behavior is displayed universally in glass systems, and the characteristic parameters associated with these functions were reasonable.

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  • Received 28 October 2020
  • Accepted 25 May 2021
  • Corrected 18 February 2022

DOI:https://doi.org/10.1103/PhysRevB.103.224408

©2021 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied PhysicsNonlinear Dynamics

Corrections

18 February 2022

Correction: A minor typographical error in Eq. (4) has been fixed.

Authors & Affiliations

T. Naka1,*, T. Nakane1, S. Ishii2, M. Nakayama1, A. Ohmura3, F. Ishikawa3, A. de Visser4, H. Abe5, and T. Uchikoshi1

  • 1National Institute for Materials Science, 1-2-1, Sengen, Tsukuba, Ibaraki 305-0047, Japan
  • 2Department of Physics, Tokyo Denki University, Hatoyama, Saitama 350-0394, Japan
  • 3Faculty of Science, Niigata University, Niigata, 950-2181, Japan
  • 4Van der Waals–Zeeman Institute, Institute of Physics, University of Amsterdam, Science Park 904, 1098 XH, Netherlands
  • 5Joint and Welding Research Institution, Osaka University, 11-1 Mihogaoka, Ibaraki, Osaka 567-0047, Japan

  • *naka.takashi@nims.go.jp

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Issue

Vol. 103, Iss. 22 — 1 June 2021

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Images

  • Figure 1
    Figure 1

    (a) Spinel structure. Red, yellow, and gray spheres represent the tetrahedral, octahedral cation, and oxygen sites, respectively. Orange and blue dashed lines are connected between nearest and next-nearest neighbor A-A pairs. Red and black dashed lines represent nearest neighbor A-B and B-B pairs, respectively. (b) Schematic phase diagrams of the AB2O4 magnet projected into the η(x)-T [6, 8] and (J2/J1)-T [2] planes.

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  • Figure 2
    Figure 2

    X-ray diffraction profiles for (a) CoGa2O4 and (b) ZnGa2O4. Note that the x-ray wavelengths used for CoGa2O4 and ZnGa2O4 are slightly different. The vertical green lines show positions of the Bragg reflections. The difference between observed and calculated intensities is plotted as the lower blue trace.

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  • Figure 3
    Figure 3

    Temperature dependence of (a) magnetic susceptibility χmol and (b) reciprocal susceptibility 1/χmol for CoGa2O4.

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  • Figure 4
    Figure 4

    Real (χ′) and imaginary (χ″) components of the ac susceptibility as a function of temperature at various frequencies.

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  • Figure 5
    Figure 5

    Semilogarithmic plot of frequency ν versus 1/Tf (Arrhenius plot) and 1/(TfT0) (Vogel-Fulcher plot). Dashed and solid lines represent least squares fitting curves of the Arrhenius function at high frequencies and the Vogel-Fulcher function, respectively.

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  • Figure 6
    Figure 6

    MTRM and (1/MTRM)(dMTRM/dT) as a function of temperature.

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  • Figure 7
    Figure 7

    (a) Decay profiles and (b) temperature dependence of the relaxation rate [MTRM(tf)MTRM(ti)]/MTRM(ti) of thermoremanent magnetization MTRM. Red solid line is a guide to aid visualization. Blue solid line represents a fitting curve to an Arrhenius function (see text).

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  • Figure 8
    Figure 8

    Isothermal decays of MTRM measured at (a) T=2 K and (b) 8.5 K. The red, blue, and green dashed lines represent curves obtained by least squares fitting of the Weron, Ogielski, and Kohlrausch relaxation functions, respectively.

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  • Figure 9
    Figure 9

    Temperature dependences of (a) ptot=p0+p1, (b) β, and (c) k and q. Dashed curve in (a) represents a numerically fitted curve that corresponds to ptot(T)=ptot0(1T/TSG)α with ptot0=4.4emu/mol and α = 0.77. Vertical and horizontal dashed lines in (c) indicate q=5/3 and T=TSG, respectively.

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  • Figure 10
    Figure 10

    Relaxation time τ as a function of TSG/T.  τac is obtained by a least squares fitting ac-χ(ν). τD and τW are obtained by numerical fittings of the decay curve of MTRM(t) with Debye and Weron relaxation functions, respectively. Inset shows τVF, τArr, and τtot as a function of TSG/T represented by red and blue solid lines and a black dotted line, respectively.

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  • Figure 11
    Figure 11

    FT IR spectra for CoGa2O4 and the isostructural compound ZnGa2O4. Arrows indicate the broad peak and shoulder observed at 560 and 720cm1, respectively.

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  • Figure 12
    Figure 12

    (a) Temperature variations of Cmol/T for CoGa2O4 and the isostructural compound ZnGa2O4. Red and black lines represent Clattice/T obtained by least squares fitting to the Einstein-Debye model for CoGa2O4 and ZnGa2O4, respectively. (b) Black open circles show the magnetic component ΔCmol/T=[Cmol(CoGa2O4)Clattice]/T. The magnetic entropy Smag is also depicted. The dashed line represents a power law with respect to temperature ΔCmol/T=0.054T0.82. (c) The temperature derivative of ΔCmol as a function of temperature. Arrow indicates the spin-glass transition point TSG. The dashed red line shows T2 variation above TSG.

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  • Figure 13
    Figure 13

    Logarithmic plot of relaxation time τac as a function of reduced temperature t=(TfTSG)/TSG. Solid line represents the results of a least squares fit to the data.

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  • Figure 14
    Figure 14

    Relaxation rate R(t) as a function of logarithmic time lnt at various waiting times. Solid line is a guide to facilitate visualization.

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