doi:10.1088/2752-5724/ad4a93

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Synthesis, disorder and Ising anisotropy in a new spin liquid candidate PrMgAl₁₁O₁₉

doi: 10.1088/2752-5724/ad4a93

1.
Key Lab for Magnetism and Magnetic Materials of the Ministry of Education, Lanzhou University, Lanzhou 730000, People’s Republic of China
2.
Songshan Lake Materials Laboratory, Dongguan, Guangdong 523808, People’s Republic of China
3.
Institute of Physics, Chinese Academy of Sciences, Beijing 100190, People’s Republic of China
4.
Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, United States of America
5.
School of Physics and Wuhan National High Magnetic Field Center, Huazhong University of Science and Technology, Wuhan 430074, People’s Republic of China

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Corresponding author: E-mail: gardnerjs@ornl.gov; E-mail: tianzhaoming@hust.edu.cn; E-mail: zweili@lzu.edu.cn; E-mail: hjguo@sslab.org.cn

摘要

Abstract: AbstractHere we report the successful synthesis of large single crystals of triangular frustrated PrMgAl₁₁O₁₉ using the optical floating zone technique. Single crystal x-ray diffraction (XRD) measurements unveiled the presence of quenched disorder within the mirror plane, specifically ~7% of Pr ions deviating from the ideal 2d site towards the 6h site. Magnetic susceptibility measurements revealed an Ising anisotropy with the c-axis being the easy axis. Despite a large spin-spin interaction that develops below ~10 K and considerable site disorder, the spins do not order or freeze down to at least 50 mK. The availability of large single crystals offers a distinct opportunity to investigate the exotic magnetic state on a triangular lattice with an easy axis out of the plane.
- spin liquid /
- disorder /
- frustration /
- triangular lattice /
- Ising anisotropy
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Figure 1. The crystal structure of PrMgAl₁₁O₁₉ extracted from single-crystal XRD refinement. Green—Pr; grey—Al; red—O; orange—Mg. The mirror plane including the disordered Pr ions is depicted in the right panel.

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Figure 2. X-ray studies of PrMgAl₁₁O₁₉. (a) A Laue pattern with the x-ray beam approximately along the c axis. The inset shows a photo of the as-grown single crystal. (b)-(d) Precession images within the HK0, 0KL and H0L planes constructed from the single-crystal XRD measurements.

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Figure 3. Temperature and field dependence of the dynamic susceptibility of PrMgAl₁₁O₁₉. (a) Temperature dependence of the magnetic susceptibility measured with the magnetic fields applied along the reciprocal a and c directions. (b) Temperature dependence of the inverse susceptibility, $χ_{c}^{- 1} (T)$ . The red and blue curves are according to the CEF fit and Curie-Weiss fit, respectively. The inset highlights the low-temperature region. (c) Temperature dependence of the real component of the ac susceptibility, $χ_{c}^{'}$ (T), measured at various frequencies. (d) Isothermal magnetization measured at various temperatures. The solid lines represent the magnetization calculated from the CEF parameters.

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Figure 4. Heat capacity from hexaaluminate single crystals. (a) $C_{p} / T$ versus T measured under various magnetic fields. The dashed line represents the phonon contribution obtained from the nonmagnetic counterpart LaMgAl₁₁O₁₉. (b) The magnetic specific heat is obtained by subtracting the phonon contributions (LaMgAl₁₁O₁₉) from the data of PrMgAl₁₁O₁₉. The red line represents a fit, $C_{m} = A T^{α}$ , to the zero field data in the temperature range between 0.2 and 2 K, with α = 1.91(1). (c) Representative change of the magnetic entropy in zero field. (d) Temperature dependence of the magnetic specific heat for NdMgAl₁₁O₁₉ together with a two-level Schottky fit. The inset shows the evolution of the gap as a function of the applied magnetic fields. A fit of $Δ = g_{c} μ_{B} H$ to the gap yields g_c of 3.92.

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Table 1. Experimental conditions for the single crystal XRD measurements, and agreement factors for the refinement.

Formula	PrMgAl₁₁O₁₉
Space group	$P 6_{3} / m m c$ (No. 194)
a, b (Å)	5.587 00(10)
c (Å)	21.8732(6)
V (Å³)	591.29(2)
Z	2
2Θ (°)	3.72 - 82.16
No. of reflections, $R_{int}$	125 34, 4.11%
No. of independent reflections	614
No. of parameters	48
Index ranges	-9 $⩽$ H $⩽$ 10,
	-10 $⩽$ K $⩽$ 10,
	-39 $⩽$ L $⩽$ 39
R, wR₂^a	1.69%, 4.60%
Goodness of fit on F²	1.42
Largest difference peak/hole (e/Å³)	0.34/-0.38

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Table 2. Refined crystal structure parameters.

Atom	occ.	x	y	z
Pr1 (2d)	0.928(10)	1/3	2/3	0.75
Pr2 (6 h)	0.024(3)	0.271(5)	0.729(5)	0.75
Al1 (2a)	1	0	0	0
Al2 (4f)	1	1/3	2/3	0.189 98(4)
Al3 (4f)	0.5	1/3	2/3	0.472 75(4)
Mg (4f)	0.5	1/3	2/3	0.472 75(4)
Al4 (12k)	1	0.167 38(4)	0.334 77(9)	0.608 39(2)
Al5 (4e)	0.5	0	0	0.2428(3)
O1 (6 h)	1	0.181 22(15)	0.3624(3)	0.25
O2 (12k)	1	0.152 14(11)	0.3043(2)	0.446 09(6)
O3 (12k)	1	-0.0112(2)	0.494 42(11)	0.348 08(5)
O4 (4f)	1	1/3	2/3	0.558 37(10)
O5 (4e)	1	0	0	0.348 18(9)

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Synthesis, disorder and Ising anisotropy in a new spin liquid candidate PrMgAl₁₁O₁₉

doi: 10.1088/2752-5724/ad4a93

Corresponding author: E-mail: gardnerjs@ornl.gov; E-mail: tianzhaoming@hust.edu.cn; E-mail: zweili@lzu.edu.cn; E-mail: hjguo@sslab.org.cn

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Synthesis, disorder and Ising anisotropy in a new spin liquid candidate PrMgAl11O19

doi: 10.1088/2752-5724/ad4a93

Corresponding author: E-mail: gardnerjs@ornl.gov; E-mail: tianzhaoming@hust.edu.cn; E-mail: zweili@lzu.edu.cn; E-mail: hjguo@sslab.org.cn

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Synthesis, disorder and Ising anisotropy in a new spin liquid candidate PrMgAl₁₁O₁₉