Antiferromagnetic long-range order in the $5{d}^{1}$ double-perovskite ${\mathrm{Sr}}_{2}{\mathrm{MgReO}}_{6}$

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Antiferromagnetic long-range order in the $5 d^{1}$ double-perovskite ${Sr}_{2} {MgReO}_{6}$

Shang Gao, Daigorou Hirai, Hajime Sagayama, Hiroyuki Ohsumi, Zenji Hiroi, and Taka-hisa Arima

Phys. Rev. B 101, 220412(R) – Published 29 June 2020

Abstract

The double-perovskite $A_{2} B B^{'} O_{6}$ with heavy transition metal ions on the ordered $B^{'}$ sites is an important family of compounds to study the interplay between electron correlation and spin-orbit coupling. Here we prepared high-quality ${Sr}_{2} {MgReO}_{6}$ powder and single-crystal samples and performed nonresonant and resonant synchrotron x-ray diffraction experiments to investigate its magnetic ground state. By combining the magnetic susceptibility and heat capacity measurements, we conclude that ${Sr}_{2} {MgReO}_{6}$ exhibits a layered antiferromagnetic order at temperatures below $\sim 55$ K with a propagation vector $q = (001)$ , which contrasts the previously suspected spin-glass state. Our works clarify the magnetic order in ${Sr}_{2} {MgReO}_{6}$ and demonstrate it as a candidate system to look for magnetic octupolar orders and exotic spin dynamics.

Received 5 April 2020
Revised 7 June 2020
Accepted 9 June 2020

DOI:https://doi.org/10.1103/PhysRevB.101.220412

Physics Subject Headings (PhySH)

Magnetic order Spin-orbit coupling

Perovskites Strongly correlated systems

DC susceptibility measurements Resonant elastic x-ray scattering Specific heat measurements X-ray diffraction

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Shang Gao^1,*, Daigorou Hirai^2,†, Hajime Sagayama³, Hiroyuki Ohsumi⁴, Zenji Hiroi², and Taka-hisa Arima^1,5

¹RIKEN Center for Emergent Matter Science, Wako 351-0198, Japan
²Institute for Solid State Physics, University of Tokyo, Kashiwa 277-8581, Japan
³Institute of Materials Structure Science, High Energy Accelerator Research Organization, Tsukuba 305-0801, Japan
⁴RIKEN SPring-8 Center, Sayo 679-5148, Japan
⁵Department of Advanced Materials Science, University of Tokyo, Kashiwa 277-8561, Japan

^*Present address: Materials Science & Technology Division and Neutron Science Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA; shang.gao@riken.jp
^†dhirai@issp.u-tokyo.ac.jp

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Vol. 101, Iss. 22 — 1 June 2020

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Figure 1
(a) Crystal structure of ${Sr}_{2} {MgReO}_{6}$ . The ${MgO}_{6}$ and ${ReO}_{6}$ octahedra are shown explicitly. (b) Refinement result of the synchrotron x-ray diffraction data measured at room temperature for the ${Sr}_{2} {MgReO}_{6}$ polycrystalline sample. Data points are shown as red circles. The calculated pattern is shown as the black solid line. The vertical bars show the positions of the Bragg peaks for ${Sr}_{2} {MgReO}_{6}$ . The blue line at the bottom shows the difference of measured and calculated intensities. Inset is the ${Sr}_{2} {MgReO}_{6}$ structure viewed along the $c$ axis. (c),(d) $T$ dependence of the lattice constants (c) and Re-O bond lengths (d).
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Figure 2
(a) X-ray oscillation photograph of ${Sr}_{2} {MgReO}_{6}$ collected at $\sim 38$ K. Inset shows the zoomed-in region around the $(- 8 - 1 - 1)$ reflection. (b) Comparison between the observed intensities at $T = 300$ K and the calculated intensities assuming a tetragonal $I 4 / m$ structure. (c) $T$ dependence of the thermal factors $U_{11}$ and $U_{33}$ for O1. Insets plot the thermal ellipsoids for the six $O^{2 -}$ ions around ${Re}^{6 +}$ at 300 (right) and 38 K (left).
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Figure 3
(a) Left axis shows the $T$ dependence of the magnetic susceptibility $χ (T)$ measured in zero-field cooling (ZFC; filled circles) and 7 T field cooling (FC; crosses). The applied field is 7 T. Right axis shows the $T$ dependence of the reversed magnetic susceptibility measured in ZFC (empty squares). Blue solid line is fit to the Curie-Weiss law. Measurements were performed on a polycrystalline sample. (b) $T$ dependence of the heat capacity $C_{p}$ . Inset plots the zoomed-in region around 55 K. (c) $χ (T)$ measured in a low field of 100 and 500 Oe. The 100 Oe data is offset by $- 1.5 \times 10^{- 4}$ emu/ $mol Oe$ for clarity. (d) Field dependence of the magnetization $M (H)$ measured at $T = 2$ K.
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Figure 4
(a) Energy dependence of the intensity for the (221) reflection around the Re $L_{3}$ edge measured at $\sim 6$ K (red circles). The black solid line is the x-ray absorption spectrum. (b) Polarization analysis of the scattered intensities around (221). $θ_{A}$ is the angle of the analyzer. (c) $T$ dependence of the intensity for the (221) reflection. The solid line is a fit to a power law, where the integrated intensities are proportional to ${(T_{N} - T)}^{η}$ with $T_{N} = 52.5 (2)$ and $η = 0.38 (2)$ . (d) Azimuthal angle $Ψ$ dependence of the intensity for the (320) reflection measured at $\sim 6$ K. Solid line is the fit to the $A {sin}^{2} Ψ + C$ relation. Inset plots a representative magnetic structure with the ${Re}^{6 +}$ moments in the $a b$ plane.
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Figure 5
Re-O-O-Re exchange paths for the AF (a) and FM (b) couplings between the nearest-neighboring ${Re}^{6 +}$ ions. This figure is adapted from Ref. [10].
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Physical Review B

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Antiferromagnetic long-range order in the $5 d^{1}$ double-perovskite ${Sr}_{2} {MgReO}_{6}$

Shang Gao, Daigorou Hirai, Hajime Sagayama, Hiroyuki Ohsumi, Zenji Hiroi, and Taka-hisa Arima

Phys. Rev. B 101, 220412(R) – Published 29 June 2020

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Physical Review B

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Antiferromagnetic long-range order in the 5d1 double-perovskite Sr2MgReO6

Shang Gao, Daigorou Hirai, Hajime Sagayama, Hiroyuki Ohsumi, Zenji Hiroi, and Taka-hisa Arima

Phys. Rev. B 101, 220412(R) – Published 29 June 2020

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Antiferromagnetic long-range order in the $5 d^{1}$ double-perovskite ${Sr}_{2} {MgReO}_{6}$