Quantum antiferromagnet bluebellite comprising a maple-leaf lattice made of spin-$1/2\phantom{\rule{0.16em}{0ex}}{\mathrm{Cu}}^{2+}$ ions

Quantum antiferromagnet bluebellite comprising a maple-leaf lattice made of spin- $1 / 2 {Cu}^{2 +}$ ions

Yuya Haraguchi, Akira Matsuo, Koichi Kindo, and Zenji Hiroi

Phys. Rev. B 104, 174439 – Published 29 November 2021

Abstract

Spin-1/2 maple-leaf lattice antiferromagnets are expected to show interesting phenomena originating from frustration effects and quantum fluctuations. We report the hydrothermal synthesis of a powder sample of bluebellite ${Cu}_{6} I O_{3} {(OH)}_{10} Cl$ as a first potential candidate. Magnetization and heat capacity measurements reveal moderate frustration with a Curie-Weiss temperature of $- 35 K$ , and a magnetic transition at $T_{N} = 17 K$ . Surprisingly, the magnetic susceptibility and heat capacity above $T_{N}$ are well reproduced by the Bonner-Fisher model, which suggests that a one-dimensional spin correlation with a magnetic interaction of 25 K occurs in the apparently two-dimensional lattice. This emergent one-dimensionality cannot be explained by orbital ordering or dimensional reduction due to geometrical frustration. We believe that there is an unknown mechanism to cause one-dimensionality in the spin-1/2 maple-leaf lattice antiferromagnet.

Received 20 April 2021
Revised 28 October 2021
Accepted 17 November 2021

DOI:https://doi.org/10.1103/PhysRevB.104.174439

Physics Subject Headings (PhySH)

Antiferromagnetism Frustrated magnetism Magnetic susceptibility Magnetism Specific heat

1-dimensional spin chains 2-dimensional systems Antiferromagnets Polycrystalline materials

Chemical synthesis Magnetization measurements X-ray diffraction

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Yuya Haraguchi ^1,*, Akira Matsuo², Koichi Kindo², and Zenji Hiroi²

¹Department of Applied Physics and Chemical Engineering, Tokyo University of Agriculture and Technology, Koganei, Tokyo 184-8588, Japan
²The Institute for Solid State Physics, The University of Tokyo, Kashiwa, Chiba 277-8581, Japan

^*chiyuya3@go.tuat.ac.jp

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Vol. 104, Iss. 17 — 1 November 2021

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Figure 1
Maple-leaf lattice with the three types of magnetic interaction $J_{d}, J_{t}$ , and $J_{h}$ for the dimers, triangles, and hexagons, respectively.
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Figure 2
(a) Powder x-ray diffraction pattern for synthetic bluebellite. The observed intensity, calculated intensity based on Rietveld analysis, and their difference are represented by red dots, black lines, and blue lines, respectively. The inset shows the crystal structure of bluebellite viewed along the layers visualized using the vesta program [21]. (b) Arrangement of atoms in a layer. (c) Arrangement of spin-carrying Cu- $3 d (x^{2} - y^{2})$ orbitals. Blue and red lobes represent the $d (x^{2} - y^{2})$ orbitals on the Cu1 and Cu2 sites, respectively. Five types of nearest-neighbor interaction are shown: $J_{t 1}$ (blue), $J_{t 2}$ (red), $J_{d}$ (black), $J_{h 1}$ (green), and $J_{h 2}$ (pink).
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Figure 3
(a) Temperature dependence of the magnetic susceptibility $M / H$ and its inverse for a polycrystalline sample of bluebellite measured under an applied magnetic field of 50 mT. The $M / H$ data after the subtraction of the low-temperature Curie-tail contribution are also shown. The dashed lines on the M/H and H/M data represent fits to the Bonner-Fisher (BF) [23] and Curie-Weiss (CW) models, respectively. (b) Temperature dependencies of $M / H$ measured at magnetic fields of 0.05, 1, 3, and 7 T. Magnetic ordering is observed at $T_{N} = 17 K$ , where the derivative of the $M / H$ curve at 1 T shows a peak and field dependence starts to appear. The inset shows the $M - H$ curve (red) and its derivative (blue) measured at 1.8 K. The black arrows indicate spin flop transitions at ±1.7 T.
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Figure 4
Temperature dependencies of heat capacity divided by temperature $C / T$ and magnetic entropy $S_{mag}$ for bluebellite. Red circles (filled and open for $μ_{0} H = 0$ and 7 T, respectively) and dashed line represent the data and lattice contribution estimated by fitting the data above 100 K $(C_{lattice} / T)$ , respectively. The black arrow indicates the magnetic transition temperature $T_{N}$ . The inset in the top panel shows a plot of $C / T$ against $T^{2}$ revealing the presence of a large $T$ -linear contribution in $C$ . Magnetic entropy $S_{mag}$ approaches $R \ln 2$ at high temperatures. The inset in the bottom panel shows the magnetic heat capacity $C_{mag}$ after the subtraction of $C_{lattice}$ . The broken line is a fit to the BF model, which yields $J$ = 25 K.
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Figure 5
Magnetization curve and its derivative measured at 4.2 K under pulsed magnetic fields up to 61.7 T for bluebellite. The magnitudes are calibrated to the data measured under static fields up to 7 T (black circles). The saturated magnetization $M_{sat}$ is $g S$ with a $g$ value of 2.27, which was obtained from the CW fitting.
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Physical Review B

covering condensed matter and materials physics

Quantum antiferromagnet bluebellite comprising a maple-leaf lattice made of spin- $1 / 2 {Cu}^{2 +}$ ions

Yuya Haraguchi, Akira Matsuo, Koichi Kindo, and Zenji Hiroi

Phys. Rev. B 104, 174439 – Published 29 November 2021

Abstract

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Physical Review B

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Quantum antiferromagnet bluebellite comprising a maple-leaf lattice made of spin-1/2Cu2+ ions

Yuya Haraguchi, Akira Matsuo, Koichi Kindo, and Zenji Hiroi

Phys. Rev. B 104, 174439 – Published 29 November 2021

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Quantum antiferromagnet bluebellite comprising a maple-leaf lattice made of spin- $1 / 2 {Cu}^{2 +}$ ions