Antiferromagnetic Order and Spin-Canting Transition in the Corrugated Square Net Compound Cu3(TeO4)(SO4)·H2O

Published

July 19, 2021

Author(s)

Zhi-Cheng Wang, Kulatheepan Thanabalasingam, Jan P. Scheifers, Alenna Streeter, Gregory T. McCandless, Jonathan N. Gaudet, Craig Brown, Carlo U. Segre, Julia Y. Chan, Fazel Tafti

Abstract

Strongly correlated electrons in layered perovskite structures have been the birthplace of high-temperature superconductivity, spin liquid, and quantum criticality. Specifically, the cuprate materials with layered structures made of corner sharing square planar CuO₄ units have been intensely studied due to their Mott insulating grounds state which leads to high-temperature superconductivity upon doping. Identifying new compounds with similar lattice and electronic structures has become a challenge in solid state chemistry. Here, we report the hydrothermal crystal growth of a new copper tellurite sulfate Cu₃(TeO₄)(SO₄)·H₂O, a promising alternative to layered perovskites. The orthorhombic phase (space group Pnma) is made of corrugated layers of corner-sharing CuO₄ square-planar units that are edge-shared with TeO₄ units. The layers are linked by slabs of corner-sharing CuO₄ and SO₄. Using both the bond valence sum analysis and magnetization data, we find purely Cu²⁺ ions within the layers, but a mixed valence of Cu²⁺/Cu⁺ between the layers. Cu₃(TeO₄)(SO₄)·H₂O undergoes an antiferromagnetic transition at T_N=67 K marked by a peak in the magnetic susceptibility. Upon further cooling, a spin-canting transition occurs at T*=12 K evidenced by a kink in the heat capacity. The spin-canting transition is explained based on a J₁-J₂ model of magnetic interactions, which is consistent with the slightly different in-plane super-exchange paths. We present Cu₃(TeO₄)(SO₄)·H₂O as a promising platform for the future doping and strain experiments that could tune the Mott insulating ground state into superconducting or spin liquid states.

Citation

Inorganic Chemistry

Volume

60

Issue

14

Pub Type

Journals

Keywords

Chemistry, New Materials, Crystallography, Magnetism, Mott insulator

Citation

Wang, Z. , Thanabalasingam, K. , Scheifers, J. , Streeter, A. , McCandless, G. , Gaudet, J. , Brown, C. , Segre, C. , Chan, J. and Tafti, F. (2021), Antiferromagnetic Order and Spin-Canting Transition in the Corrugated Square Net Compound Cu₃(TeO₄)(SO₄)·H₂O, Inorganic Chemistry (Accessed September 15, 2024)