Geometric Frustration on the Trillium Lattice in a Magnetic Metal-Organic Framework

Bulled, Johnathan M.; Paddison, Joseph A. M.; Wildes, Andrew; Lhotel, Elsa; Cassidy, Simon J.; Pato-Doldán, Breogán; Gómez-Aguirre, L. Claudia; Saines, Paul J.; Goodwin, Andrew L.

doi:10.1103/physrevlett.128.177201

Title: Geometric Frustration on the Trillium Lattice in a Magnetic Metal-Organic Framework

Journal Article · Tue Apr 26 00:00:00 EDT 2022 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.128.177201· OSTI ID:1869123

^[1]; Paddison, Joseph A. M. ^[2];

^[3]; Lhotel, Elsa ^[4]; Cassidy, Simon J. ^[1];

^[5];

^[6];

^[7]; Goodwin, Andrew L. ^[1]

Univ. of Oxford (United Kingdom). Inorganic Chemistry Lab.
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Cambridge (United Kingdom)
Inst. Laue-Langevin (ILL), Grenoble (France)
Institut Néel, Grenoble (France)
Univ. of Bergen (Norway)
University of A Coruña (Spain)
Univ. of Kent, Canterbury (United Kingdom)

In the dense metal-organic framework $Na [Mn {(HCOO)}_{3}]$ , ${Mn}^{2 +}$ ions ( $S = \frac{5}{2}$ ) occupy the nodes of a “trillium” net. In this work, we show that the system is strongly magnetically frustrated: the Néel transition is suppressed well below the characteristic magnetic interaction strength; short-range magnetic order persists far above the Néel temperature; and the magnetic susceptibility exhibits a pseudo-plateau at $\frac{1}{3}$ -saturation magnetization. A simple model of nearest-neighbor Heisenberg antiferromagnetic and dipolar interactions accounts quantitatively for all observations, including an unusual 2- $k$ magnetic ground state. We show that the relative strength of dipolar interactions is crucial to selecting this particular ground state. Geometric frustration within the classical spin liquid regime gives rise to a large magnetocaloric response at low applied fields that is degraded in powder samples as a consequence of the anisotropy of dipolar interactions.

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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); European Research Council (ERC); Engineering and Physical Sciences Research Council (EPSRC); Leverhulme Trust; European Union Horizon 2020

Grant/Contract Number:: AC05-00OR22725; 788144; EP/T027886/1; RPG-2018-268; 824109

OSTI ID:: 1869123

Journal Information:: Physical Review Letters, Vol. 128, Issue 17; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Geometric Frustration on the Trillium Lattice in a Magnetic Metal-Organic Framework

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