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

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

doi:10.1039/d2qm01272c

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

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

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

Abstract

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. 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.

Original language	English
Pages (from-to)	1058-1071
Number of pages	14
Journal	Materials Chemistry Frontiers
Volume	7
Issue number	6
DOIs	https://doi.org/10.1039/d2qm01272c
State	Published - Feb 13 2023

Funding

This research used resources at the Missouri University Research Reactor (MURR). This work was supported in part by a University of Missouri Research Council Grant (Grant Number: URC-22-021). The research at the Oak Ridge National Laboratory (ORNL) is supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division. This research used resources at the High Flux Isotope Reactor and Spallation Neutron Source, DOE Office of Science User Facilities operated by ORNL. The synthesis, X-ray diffraction and crystal growth at Clemson University was supported by awards from the NSF DMR - 1808371 and DMR - 2219129. This research used resources at the Missouri University Research Reactor (MURR). This work was supported in part by a University of Missouri Research Council Grant (Grant Number: URC-22-021). The research at the Oak Ridge National Laboratory (ORNL) is supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division. This research used resources at the High Flux Isotope Reactor and Spallation Neutron Source, DOE Office of Science User Facilities operated by ORNL. The synthesis, X-ray diffraction and crystal growth at Clemson University was supported by awards from the NSF DMR – 1808371 and DMR – 2219129.

Funders	Funder number
High Flux Isotope Reactor and Spallation Neutron Source
University of Missouri Research Council	URC-22-021
National Science Foundation	DMR – 2219129, DMR – 1808371
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
University of Missouri
Division of Materials Sciences and Engineering

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@article{1f4829be977d4bf09122f3fa39d979a7,

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

abstract = "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 Jbb and Jbv magnetic exchange. The magnetism is highly anisotropic with the b-axis (chain) along the easy axis and the material orders antiferromagnetically at TN = 5 K. There are two successive metamagnetic transitions, the first at Hc1 = 0.2 kOe into a ferrimagnetic structure, and the other at Hc2 = 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. 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 Jbb = 0.028 meV and Jbv = 0.13 meV, while the interchain exchange parameter is considerably weaker at Jch = (0.0047/Nch) 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.",

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

note = "Publisher Copyright: {\textcopyright} 2023 The Royal Society of Chemistry.",

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doi = "10.1039/d2qm01272c",

language = "English",

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T1 - Field tunable magnetic transitions of CsCo2(MoO4)2(OH)

T2 - a triangular chain structure with a frustrated geometry

AU - Sanjeewa, Liurukara D.

AU - Garlea, V. Ovidiu

AU - Fishman, Randy S.

AU - Foroughian, Mahsa

AU - Yin, Li

AU - Xing, Jie

AU - Parker, David S.

AU - Smith Pellizzeri, Tiffany M.

AU - Sefat, Athena S.

AU - Kolis, Joseph W.

PY - 2023/2/13

Y1 - 2023/2/13

N2 - 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 Jbb and Jbv magnetic exchange. The magnetism is highly anisotropic with the b-axis (chain) along the easy axis and the material orders antiferromagnetically at TN = 5 K. There are two successive metamagnetic transitions, the first at Hc1 = 0.2 kOe into a ferrimagnetic structure, and the other at Hc2 = 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. 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 Jbb = 0.028 meV and Jbv = 0.13 meV, while the interchain exchange parameter is considerably weaker at Jch = (0.0047/Nch) 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.

AB - 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 Jbb and Jbv magnetic exchange. The magnetism is highly anisotropic with the b-axis (chain) along the easy axis and the material orders antiferromagnetically at TN = 5 K. There are two successive metamagnetic transitions, the first at Hc1 = 0.2 kOe into a ferrimagnetic structure, and the other at Hc2 = 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. 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 Jbb = 0.028 meV and Jbv = 0.13 meV, while the interchain exchange parameter is considerably weaker at Jch = (0.0047/Nch) 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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JO - Materials Chemistry Frontiers

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

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