K2Mn3O(OH)(VO4)(V2O7) with Sawtooth Chains of MultiValent Manganese Triangular Trimer Units: Magnetic Susceptibility Shrouding a Long-Range Antiferromagnetic Order of Ferromagnetic Triangles

Yakubovich, O.; Shvanskaya, L.; Kiriukhina, G.; Simonov, S.; Volkov, A.; Dimitrova, O.; Glazkov, V.N.; Ignatenko, A.; Chung, S.H.; Koo, H.; Whangbo, M.; Vasiliev, A.N.

Авторы: Yakubovich Olga, Shvanskaya Larisa, Kiriukhina Galina, Simonov Sergey, Volkov Anatoly, Dimitrova Olga, Glazkov Vasiliy N., Ignatenko Andrey, Chung Seung Hwan, Koo Hyun-Joo, Whangbo Myung-Hwan, Vasiliev Alexander N.
Журнал: Inorganic Chemistry
Том: 62
Номер: 35
Год издания: 2023
Издательство: American Chemical Society
Местоположение издательства: United States
Первая страница: 14180
Последняя страница: 14190
DOI: 10.1021/acs.inorgchem.3c01100
Аннотация: Ortho-pyrovanadate (or ortho-diorthovanadate) K2Mn3+2Mn2+O(OH)(VO4)(V2O7) synthesized hydrothermally crystallizes in the orthorhombic space group Pnma with a = 17.9155(5), b = 5.8940(2), c = 10.9971(3) Å, V = 1161.23(6) Å3 and Z = 4. Its crystal structure features linear chains of edge-sharing Mn3+O6 octahedra with every second pair of Mn3+O6 octahedra condensed with a Mn2+O6 octahedron on the one side of a chain in a sawtooth pattern so that each sawtooth chain consists of triangular trimer. These sawtooth chains, running parallel to the b axis and linked by the VO4 and V2O7 groups, form a framework with channels populated by K atoms. The new compound is a structural analogue of the mineral zoisite, Ca2Al3O(OH)(SiO4)(Si2O7), showing a striking example of very different chemical compositions. K2Mn3O(OH)(VO4)(V2O7) undergoes a phase transition into an ordered antiferromagnetic state at TN = 14.4 K, which is detected by high frequency electron spin resonance as well as by both specific heat Cp and Fisher’s specific heat d(χT)/dT measurements. However, this phase transition is not detected by magnetic susceptibility measurements. The origin of this puzzling observation was resolved by evaluating the spin exchanges of K2Mn3O(OH)(VO4)(V2O7), which reveals that each triangular trimer is a ferromagnetically-coupled cluster, and the observed ordering involves an antiferromagnetic ordering between the ferromagnetic clusters. This ordering is shrouded in magnetic susceptibility measurements due to the susceptibility contributions from the individual ferromagnetic triangular trimers even below TN. We showed that the magnetic susceptibility of K2Mn3O(OH)(VO4)(V2O7) between 30 K and room temperature is satisfactorily described by an antiferromagnetic chain made up of ferromagnetically-coupled triangular clusters described by a few spin exchange parameters.
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K2Mn3O(OH)(VO4)(V2O7) with Sawtooth Chains of MultiValent Manganese Triangular Trimer Units: Magnetic Susceptibility Shrouding a Long-Range Antiferromagnetic Order of Ferromagnetic Trianglesстатья

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