Field tunable magnetic transitions of CsCo2(MoO4)2(OH): a triangular chain structure with a frustrated geometry

Sanjeewa, Liurukara D.; Garlea, V. Ovidiu; Fishman, Randy S.; Foroughian, Mahsa; Yin, Li; Xing, Jie; Parker, David S.; Smith Pellizzeri, Tiffany M.; Sefat, Athena S.; Kolis, Joseph W.

doi:10.1039/d2qm01272c

Title: Field tunable magnetic transitions of CsCo₂(MoO₄)₂(OH): a triangular chain structure with a frustrated geometry

Journal Article · 12 February 2023 · Materials Chemistry Frontiers

DOI: https://doi.org/10.1039/d2qm01272c · OSTI ID:1961941

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^[2]; Foroughian, Mahsa ^[3];

^[2]; Xing, Jie ^[2];

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^[2]; Kolis, Joseph W. ^[3]

Univ. of Missouri, Columbia, MO (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Clemson Univ., SC (United States)
Eastern Illinois University, Charleston, IL (United States)

The sawtooth chain compound CsCo₂(MoO₄)₂(OH) is a complex magnetic system and here, we present a comprehensive series of magnetic and neutron scattering measurements to determine its magnetic phase diagram. The magnetic properties of CsCo₂(MoO₄)₂(OH) exhibit a strong coupling to the crystal lattice and its magnetic ground state can be easily manipulated by applied magnetic fields. There are two unique Co²⁺ ions, base and vertex, with J_bb and J_bv magnetic exchange. The magnetism is highly anisotropic with the b-axis (chain) along the easy axis and the material orders antiferromagnetically at T_N = 5 K. There are two successive metamagnetic transitions, the first at H_c₁ = 0.2 kOe into a ferrimagnetic structure, and the other at H_c₂ = 20 kOe to a ferromagnetic phase. Heat capacity measurements in various fields support the metamagnetic phase transformations, and the magnetic entropy value is intermediate between S = 3/2 and 1/2 states. The zero field antiferromagnetic phase contains vertex magnetic vectors (Co(1)) aligned parallel to the b-axis, while the base vectors (Co(2)) are canted by 34° and aligned in an opposite direction to the vertex vectors. The spins in parallel adjacent chains align in opposite directions, creating an overall antiferromagnetic structure. Further, at a 3 kOe applied magnetic field, adjacent chains flip by 180° to generate a ferrimagnetic phase. An increase in field gradually induces the Co(1) moment to rotate along the b-axis and align in the same direction with Co(2) generating a ferromagnetic structure. The antiferromagnetic exchange parameters are calculated to be J_bb = 0.028 meV and J_bv = 0.13 meV, while the interchain exchange parameter is considerably weaker at J_ch = (0.0047/N_ch) meV. Our results demonstrate that the CsCo₂(MoO₄)₂(OH) is a promising candidate to study new physics associated with sawtooth chain magnetism and it encourages further theoretical studies as well as the synthesis of other sawtooth chain structures with different magnetic ions.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; University of Missouri Research Council

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1961941

Alternate ID(s):: OSTI ID: 1957657

Journal Information:: Materials Chemistry Frontiers, Journal Name: Materials Chemistry Frontiers Journal Issue: 6 Vol. 7; ISSN 2052-1537

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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