Chemical Design of Spin Frustration to Realize Topological Spin Glasses
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correction-to-chemical-design-of-spin-frustration-to-realize-topological-spin-glasses.pdf
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Correction
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Author(s)
Amtry, Stephanie
Campello, Arthur
Tong, Christopher
Puggioni, Danilo
Rondinelli, James
Lee, Young
Freedman, Danna
Date Issued
October 9, 2024
Journal
Journal of the American Chemical Society
Publisher
American Chemical Society
Citation
Chemical Design of Spin Frustration to Realize Topological Spin Glasses. Stephanie M. Amtry, Arthur C. Campello, Christopher L. Tong, Danilo Puggioni, James M. Rondinelli, Young S. Lee, and Danna E. Freedman. Journal of the American Chemical Society 2024 146 (42), 29040-29052.
Version
Author's final manuscript
Abstract
Patterning spins to generate collective behavior is at the core of condensed matter physics. Physicists develop techniques, including the fabrication of magnetic nanostructures and precision layering of materials specifically to engender frustrated lattices. As chemists, we can access such exotic materials through targeted chemical synthesis and create new lattice types by chemical design. Here, we introduce a new approach to induce magnetic frustration on a modified honeycomb lattice through a competition of alternating antiferromagnetic (AFM) and ferromagnetic (FM) nearest-neighbor interactions. By subtly modulating these two types of interactions through facile synthetic modifications, we created two systems: (1) a topological spin glass and (2) a frustrated spin-canted magnet with low-temperature exchange bias. To design this unconventional magnetic lattice, we used a metal−organic framework (MOF) platform, Ni 3 (pymca) 3 X 3 (NipymcaX where pymca = pyrimidine-2-carboxylato and X = Cl − , Br −). We isolated two MOFs, NipymcaCl and NipymcaBr, featuring canted Ni 2+-based moments. Despite this similarity, differences in the single-ion anisotropies of the Ni 2+ spins result in magnetic properties for each material. NipymcaCl is a topological spin glass, while NipymcaBr is a rare frustrated magnet with low-temperature exchange bias. Density functional theory calculations and Monte Carlo simulations on the NipymcaX lattice support the presence of magnetic frustration as a result of alternating AFM and FM interactions. Our calculations enabled us to determine the ground-state spin configuration and the distribution of spin−spin correlations relative to paradigmatic kagoméand triangular lattices. This modified honeycomb lattice is similar to the electronic Kekule-O phase in graphene and provides a highly tunable platform to realize unconventional spin physics.
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DOI of Published Version
https://doi.org/10.1021/jacs.4c10113
