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Field-induced successive phase transitions in the J1−J2 buckled honeycomb antiferromagnet Cs3Fe2Cl9

Y. Ishii, Y. Narumi, Y. Matsushita, M. Oda, T. Kida, M. Hagiwara, and H. K. Yoshida
Phys. Rev. B 103, 104433 – Published 25 March 2021
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  • INTRODUCTION
  • EXPERIMENTS
  • RESULTS
  • DISCUSSION
  • CONCLUSION
  • ACKNOWLEDGMENTS
    • Supplemental Material
    References

    Abstract

    The magnetic properties of Cs3Fe2Cl9 single crystals were investigated by magnetic and thermal measurements. The crystal structure of Cs3Fe2Cl9 consists of a bilayer triangular lattice of Fe3+ ions. The analysis of magnetic susceptibility clarified that the intra- and interdimer interactions are comparable with each other, and Cs3Fe2Cl9 is regarded as a spin-5/2 J1−J2 buckled honeycomb antiferromagnet with the ferromagnetic interlayer interaction J3. The susceptibility for the magnetic field H||c axis exhibits a sudden drop at the Néel temperature TN=5.4K, indicating a first-order magnetic phase transition. One of the characteristic features is the linear temperature dependence below TN. Furthermore, Cs3Fe2Cl9 undergoes successive magnetic phase transitions in high magnetic fields along the c axis. We obtained a rich H-T phase diagram in which the Ms/2 magnetization-plateau phase is included. These unique magnetic behaviors probably originate from the competition of magnetic interactions and the easy-axis anisotropy in the antiferromagnetic J1−J2 buckled honeycomb network.

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    • Received 23 July 2020
    • Revised 15 February 2021
    • Accepted 17 February 2021

    DOI:https://doi.org/10.1103/PhysRevB.103.104433

    ©2021 American Physical Society

    Physics Subject Headings (PhySH)

    1. Research Areas
    AntiferromagnetismFrustrated magnetismMagnetic interactionsMagnetic orderMagnetic phase transitionsMagnetic susceptibility
    Condensed Matter, Materials & Applied Physics

    Authors & Affiliations

    Y. Ishii1, Y. Narumi2, Y. Matsushita3, M. Oda4, T. Kida2, M. Hagiwara2, and H. K. Yoshida4

    • 1Department of Physics, Graduate School of Science, Hokkaido University, Sapporo 060-0810, Japan
    • 2Center for Advanced High Magnetic Field Science, Graduate School of Science, Osaka University, Toyonaka, Osaka 560-0043, Japan
    • 3National Institute for Materials Science, Tsukuba, Ibaraki 305-0044, Japan
    • 4Department of Physics, Faculty of Science, Hokkaido University, Sapporo, Hokkaido 060-0810, Japan

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    Vol. 103, Iss. 10 — 1 March 2021

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    Images

    • Figure 1
      Figure 1

      (a) Schematic illustration of the bilayer triangular lattice. Red and green spheres represent magnetic ions. The interactions J1, J2, and J3 are the interactions of the interbilayer triangular lattice plane, within the triangular lattice, and the intertriangular lattice within the bilayers, respectively. (b) Projection of the buckled honeycomb network onto the ab plane.

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    • Figure 2
      Figure 2

      (a) Perspective view of the crystal structure of A3M2X9. (b) Triangular lattice plane made from the Fe2Cl9 dimer along the c direction. Cs ions are not shown for ease of viewing. (c) Three dominant interactions J1, J2, and J3 corresponding to those of the bilayer triangular lattice shown in Fig. 1. The intradimer Fe-Fe distance d3, angle of intradimer Fe-Cl-Fe θ1, and interdimer Cl-Cl distances d1 and d2 are illustrated. (d) Photo of a single crystal of Cs3Fe2Cl9.

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    • Figure 3
      Figure 3

      Temperature dependence of magnetic susceptibilities of Cs3Fe2Cl9 for H||c axis (a) and H||ab plane (b). Open circles (gray) and red broken lines represent the experimental results and the results of the tenth-order high-temperature expansion [38], respectively. Open squares (gray) and blue solid lines show the inverse susceptibilities and their Curie-Weiss fittings above 50 K, respectively.

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    • Figure 4
      Figure 4

      Temperature dependence of magnetic susceptibilities for H||c axis and H||ab plane measured at 1 T. Dotted line for the H||c axis data is guide for the eyes for the linear T dependence of the susceptibility.

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    • Figure 5
      Figure 5

      Temperature dependence of magnetic susceptibilities in various magnetic fields below 8 K for H||c axis. For all plots, circles and triangles are the zero field cooling and field cooling data, respectively. Black solid triangles indicate the transition temperatures determined by the differentials of the magnetic susceptibilities (Fig. S4 in the Supplemental Material [37]) and the heat capacities. Data are shifted upward by 0.01emumolFe–1 as an offset.

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    • Figure 6
      Figure 6

      Temperature dependence of magnetic susceptibilities at various magnetic fields below 8 K for H||ab plane. For all plots, circles and triangles are the zero field cooling and field cooling data, respectively. Arrows indicate the transition temperatures. Data are shifted upward by 0.005emumolFe–1 as an offset.

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    • Figure 7
      Figure 7

      [(a)–(c)] Magnetization curves (left axis) for the H||c axis measured in magnetic fields of up to 7 T and field differentials dM/dH (right axis) with increasing and decreasing field. Solid lines and broken lines represent dM/dH with increasing and decreasing field, respectively. Data in [(a)–(c)] are shifted upward by 1.0μBFe–1 as an offset. Transition fields H2c and H4c were determined by taking the middle point of the hysteresis at each temperature. (d) Magnetization curves and dM/dH for the H||ab plane measured in magnetic fields of up to 7 T. Data in (d) are also shifted upward by 1.0μBFe–1 as an offset.

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    • Figure 8
      Figure 8

      High-field magnetization curves (blue and red lines) and field differentials dM/dH (green and orange lines) of Cs3Fe2Cl9 for (a) the H||c axis and (b) the H||ab plane. Absolute values were calibrated using the steady field data measured by MPMS. Blue (green) and red (orange) lines are the data with increasing and decreasing field, respectively. Horizontal and vertical broken lines show Ms/2 and the transition fields, respectively. H1c=2.7T, H2c=3.7T, H4c=7T, H5c=11.3T, H6c=14.5T, Hsc=17.4T, H2ab=12.4T, and Hsab=19.4T are estimated by taking the middle of the hysteresis at the transitions. The saturation magnetization value for the H||c axis is 4.9μBFe–1, and that for the H||ab plane is 4.8μBFe–1.

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    • Figure 9
      Figure 9

      [(a)–(c)] Heat capacities measured in various magnetic fields for the H||c axis. Data are normalized by the largest peak top value Cp(max) for each data series shown in the graphs (value in parentheses). (d) Enlarged figure around small peaks in 2.8, 3, 3.2, 6, and 6.5 T. Data are shown with offset by 1.0 for [(a)–(c)], and by 3.0JK–1mol–1 for (d).

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    • Figure 10
      Figure 10

      Magnetic field vs temperature phase diagram for Cs3Fe2Cl9 constructed by magnetic measurement, heat capacity measurement, and high-field magnetization data for (a) H||c axis and for (b) H||ab plane. Rhombic squares (blue), circles (orange), triangles (red), and squares (green) are the transition temperatures and fields determined from the temperature dependence of magnetic susceptibilities (MT), magnetization curves (MH), high-field magnetizations (HF), and heat capacities (HC), respectively. Bars represent the hysteresis field ranges of first-order phase transitions. Black lines are guides for the eye of phase boundaries.

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    • Figure 11
      Figure 11

      (a) Ground state (T=0) phase diagram for the S=5/2 Ising J1−J2 honeycomb antiferromagnet in a magnetic field, calculated in accordance with Ref. [44]. Critical fields determined from high-field magnetization curves at 1.4 K in Cs3Fe2Cl9 normalized by the J1 are plotted at the J2/J1=0.41 vertical line. Bars on the square marker represent the width of hysteresis of high-field magnetizations (hystereses of H1c, H3c, H5c, H6c, and Hsc are smaller than the marker size). (b,c) Candidates for the ground state spin structures of Ising J1−J2 HLAFM. In the present system, Cs3Fe2Cl9, AF II is expected to be the ground state with J2/J1=0.41 (see text). [(d),(e)] Candidates for the Ms/2 plateau of the J1−J2 HLAFM model. Open and closed circles represent up and down spins, respectively. Blue shaded regions in [(b)–(e)] correspond to the magnetic unit cell.

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