Bilayer Square Lattice Tb2SrAl2O7with Structural Z8Vortices and Magnetic Frustration

Xianghan Xu; Fei Ting Huang; Alemayehu S. Admasu; Jaewook Kim; Kefeng Wang; Erxi Feng; Huibo Cao; Sang Wook Cheong

doi:10.1021/acs.chemmater.1c03771

Bilayer Square Lattice Tb₂SrAl₂O₇with Structural Z₈Vortices and Magnetic Frustration

Xianghan Xu, Fei Ting Huang, Alemayehu S. Admasu, Jaewook Kim, Kefeng Wang, Erxi Feng, Huibo Cao, Sang Wook Cheong

Single Crystal Diffraction

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4 Scopus citations

Abstract

The bilayer perovskites' family A3B2O7 holds rich structural complexity. When magnetism freedom is added in, great opportunities appear for new physics. Magnetic Tb ions in Tb2SrAl2O7 are known to crystallize in a bilayer square lattice. The results of our comprehensive neutron, X-ray diffraction, and transmission electron microscopy (TEM) experiments reveal a crystallographic P42/mnm symmetry accompanied with room-temperature topological type-II Z8 vortex domains, whose density is controllable by cooling rates, as described by the Kibble-Zurek mechanism. The DC magnetic susceptibility without long-range order down to 1.8 K suggests frustrated magnetism, while a spin freezing <2.5 K is observed in the AC susceptibility, which is likely due to the antisite disorder and another possible cause of no long-range ordering. Strong temperature evolution of magnetic anisotropy indicates an interplay of low-lying crystal electric field levels and anisotropic exchange interactions. Our results suggest that Tb2SrAl2O7 is a promising candidate of magnetic frustration in a bilayer square lattice, and this system can be a new playground for exploring exotic magnetic states in bilayer square lattices, topological magnetic edge states at coherent crystallographic domain walls, and multifunctional applications.

Original language	English
Pages (from-to)	1225-1234
Number of pages	10
Journal	Chemistry of Materials
Volume	34
Issue number	3
DOIs	https://doi.org/10.1021/acs.chemmater.1c03771
State	Published - Feb 8 2022

Funding

The work at Rutgers University was supported by the DOE under Grant no. DOE: DE-FG02-07ER46382. The work at Oak Ridge National Laboratory was supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Early Career Research Program Award KC0402010, under Contract DE-AC05-00OR22725. This research used resources at the High Flux Isotope Reactor and the Spallation Neutron Source, the DOE Office of Science User Facility operated by ORNL. The authors thank Prof. Premala Chandra (Rutgers University) for the useful discussions.

Funders	Funder number
U.S. Department of Energy	DE-FG02-07ER46382
Office of Science
Basic Energy Sciences	DE-AC05-00OR22725, KC0402010

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10.1021/acs.chemmater.1c03771

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title = "Bilayer Square Lattice Tb2SrAl2O7with Structural Z8Vortices and Magnetic Frustration",

abstract = "The bilayer perovskites' family A3B2O7 holds rich structural complexity. When magnetism freedom is added in, great opportunities appear for new physics. Magnetic Tb ions in Tb2SrAl2O7 are known to crystallize in a bilayer square lattice. The results of our comprehensive neutron, X-ray diffraction, and transmission electron microscopy (TEM) experiments reveal a crystallographic P42/mnm symmetry accompanied with room-temperature topological type-II Z8 vortex domains, whose density is controllable by cooling rates, as described by the Kibble-Zurek mechanism. The DC magnetic susceptibility without long-range order down to 1.8 K suggests frustrated magnetism, while a spin freezing <2.5 K is observed in the AC susceptibility, which is likely due to the antisite disorder and another possible cause of no long-range ordering. Strong temperature evolution of magnetic anisotropy indicates an interplay of low-lying crystal electric field levels and anisotropic exchange interactions. Our results suggest that Tb2SrAl2O7 is a promising candidate of magnetic frustration in a bilayer square lattice, and this system can be a new playground for exploring exotic magnetic states in bilayer square lattices, topological magnetic edge states at coherent crystallographic domain walls, and multifunctional applications.",

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AU - Feng, Erxi

AU - Cao, Huibo

AU - Cheong, Sang Wook

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AB - The bilayer perovskites' family A3B2O7 holds rich structural complexity. When magnetism freedom is added in, great opportunities appear for new physics. Magnetic Tb ions in Tb2SrAl2O7 are known to crystallize in a bilayer square lattice. The results of our comprehensive neutron, X-ray diffraction, and transmission electron microscopy (TEM) experiments reveal a crystallographic P42/mnm symmetry accompanied with room-temperature topological type-II Z8 vortex domains, whose density is controllable by cooling rates, as described by the Kibble-Zurek mechanism. The DC magnetic susceptibility without long-range order down to 1.8 K suggests frustrated magnetism, while a spin freezing <2.5 K is observed in the AC susceptibility, which is likely due to the antisite disorder and another possible cause of no long-range ordering. Strong temperature evolution of magnetic anisotropy indicates an interplay of low-lying crystal electric field levels and anisotropic exchange interactions. Our results suggest that Tb2SrAl2O7 is a promising candidate of magnetic frustration in a bilayer square lattice, and this system can be a new playground for exploring exotic magnetic states in bilayer square lattices, topological magnetic edge states at coherent crystallographic domain walls, and multifunctional applications.

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Bilayer Square Lattice Tb₂SrAl₂O₇with Structural Z₈Vortices and Magnetic Frustration

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