Uncovering the S = ½ kagome ferromagnet within a family of metal–organic frameworks

Samuel A. Ivko, Katherine Tustain, Tristan Dolling, Aly Abdeldaim, Otto H. J. Mustonen, Pascal Manuel, Chennan Wang, Hubertus Luetkens, Lucy Clark*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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Abstract

Kagome networks of ferromagnetically or antiferromagnetically coupled S = ½ magnetic moments represent important models in the pursuit of a diverse array of novel quantum and topological states of matter. Here, we explore a family of Cu2+-containing metal–organic frameworks (MOFs) bearing S = ½  kagome layers pillared by ditopic organic linkers with the general formula Cu3(CO3)2(x)3·2ClO4 (MOF-x), where x is 1,2-bis(4-pyridyl)ethane (bpe), 1,2-bis(4-pyridyl)ethylene (bpy), or 4,4′-azopyridine (azpy). Despite more than a decade of investigation, the nature of the magnetic exchange interactions in these materials remained unclear, meaning that whether the underlying magnetic model is that of an S = ½ kagome ferromagnet or antiferromagnet is unknown. Using single-crystal X-ray diffraction, we have developed a chemically intuitive crystal structure for this family of materials. Then, through a combination of magnetic susceptibility, powder neutron diffraction, and muon-spin spectroscopy measurements, we show that the magnetic ground state of this family consists of S = ½  ferromagnetic kagome layers that are coupled antiferromagnetically via their extended organic pillaring linkers.
Original languageEnglish
Pages (from-to)5409–5421
Number of pages13
JournalChemistry of Materials
Volume34
Issue number12
Early online date9 Jun 2022
DOIs
Publication statusPublished - 28 Jun 2022

Bibliographical note

Funding Information:
This work was supported by the UK Engineering and Physical Sciences Research Council (EPSRC) through Grants EP/T02271X/1 and EP/V028774/1. Access to the ISIS Neutron and Muon Source was provided through the UK Science and Technology Facilities Council (STFC). The authors are grateful to L. Male (University of Birmingham) for assistance with single-crystal X-ray diffraction data collection, G. Stenning (ISIS) and M. Chung (University of Birmingham) for assistance with magnetic susceptibility data collection, and J. Graham (University of Birmingham) for assistance with data collection on WISH. O.H.J.M. is grateful for funding through Leverhulme Trust Early Career Fellowship ECF-2021-170.

Publisher Copyright:
© 2022 The Authors. Published by American Chemical Society.

ASJC Scopus subject areas

  • General Chemistry
  • General Chemical Engineering
  • Materials Chemistry

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