Strong Magnetocrystalline Anisotropy Arising from Metal–Ligand Covalency in a Metal–Organic Candidate for 2D Magnetic Order
Abstract
Layered metal-organic frameworks are promising candidates for new two-dimensional (2D) magnets, as the synthetic programmability of these materials can provide a route to diverse structural and electronic properties. However, such framework materials typically lack the heavy elements that engender magnetocrystalline anisotropy in the monolayer ferromagnets reported to date. Alternative sources of magnetic anisotropy are therefore needed in these materials. Here, we report the synthesis of single crystals of the framework material (NMe4)2[Fe2L3] (H2L = 3,6-dichloro-2,5-dihydroxybenzoquinone) and evaluate the angular dependence of its magnetic properties. Oriented-crystal magnetization measurements reveal strong uniaxial anisotropy, where the easy axis is aligned with the crystallographic c axis. While the spin carriers of this structure are isotropic S = 5/2 FeIII metal centers and S = 1/2 organic linkers, the anisotropy energy of the framework material is comparable to that of reported 2D ferromagnets. Density functional theory calculations indicate that the observed magnetocrystalline anisotropy arises from ligand-to-metal charge transfer that enhances the magnetic anisotropy of the otherwise-isotropic Fe centers, suggesting that metal-ligand covalency can be utilized as a general additive for the development of 2D magnets. These results show the possibility for (NMe4)2[Fe2L3] to retain magnetic order down to the 2D monolayer limit. In addition, themore »
- Authors:
-
- Northwestern Univ., Evanston, IL (United States)
- Univ. of California, Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Northwestern Univ., Evanston, IL (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Northwestern Univ., Evanston, IL (United States); Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- Camille and Henry Dreyfus Foundation; National Science Foundation (NSF); State of Illinois; Institute of Nanotechnology (IIN); USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1865140
- Alternate Identifier(s):
- OSTI ID: 1905576; OSTI ID: 1961803
- Grant/Contract Number:
- SC0019356; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 33; Journal Issue: 22; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Two dimensional materials; Magnetic properties; Crystals; Crystal structure; Layered materials
Citation Formats
Wang, Yiran, Ziebel, Michael E., Sun, Lei, Gish, J. Tyler, Pearson, Tyler J., Lu, Xue-Zeng, Thorarinsdottir, Agnes E., Hersam, Mark C., Long, Jeffrey R., Freedman, Danna E., Rondinelli, James M., Puggioni, Danilo, and Harris, T. David. Strong Magnetocrystalline Anisotropy Arising from Metal–Ligand Covalency in a Metal–Organic Candidate for 2D Magnetic Order. United States: N. p., 2021.
Web. doi:10.1021/acs.chemmater.1c02670.
Wang, Yiran, Ziebel, Michael E., Sun, Lei, Gish, J. Tyler, Pearson, Tyler J., Lu, Xue-Zeng, Thorarinsdottir, Agnes E., Hersam, Mark C., Long, Jeffrey R., Freedman, Danna E., Rondinelli, James M., Puggioni, Danilo, & Harris, T. David. Strong Magnetocrystalline Anisotropy Arising from Metal–Ligand Covalency in a Metal–Organic Candidate for 2D Magnetic Order. United States. https://doi.org/10.1021/acs.chemmater.1c02670
Wang, Yiran, Ziebel, Michael E., Sun, Lei, Gish, J. Tyler, Pearson, Tyler J., Lu, Xue-Zeng, Thorarinsdottir, Agnes E., Hersam, Mark C., Long, Jeffrey R., Freedman, Danna E., Rondinelli, James M., Puggioni, Danilo, and Harris, T. David. Tue .
"Strong Magnetocrystalline Anisotropy Arising from Metal–Ligand Covalency in a Metal–Organic Candidate for 2D Magnetic Order". United States. https://doi.org/10.1021/acs.chemmater.1c02670. https://www.osti.gov/servlets/purl/1865140.
@article{osti_1865140,
title = {Strong Magnetocrystalline Anisotropy Arising from Metal–Ligand Covalency in a Metal–Organic Candidate for 2D Magnetic Order},
author = {Wang, Yiran and Ziebel, Michael E. and Sun, Lei and Gish, J. Tyler and Pearson, Tyler J. and Lu, Xue-Zeng and Thorarinsdottir, Agnes E. and Hersam, Mark C. and Long, Jeffrey R. and Freedman, Danna E. and Rondinelli, James M. and Puggioni, Danilo and Harris, T. David},
abstractNote = {Layered metal-organic frameworks are promising candidates for new two-dimensional (2D) magnets, as the synthetic programmability of these materials can provide a route to diverse structural and electronic properties. However, such framework materials typically lack the heavy elements that engender magnetocrystalline anisotropy in the monolayer ferromagnets reported to date. Alternative sources of magnetic anisotropy are therefore needed in these materials. Here, we report the synthesis of single crystals of the framework material (NMe4)2[Fe2L3] (H2L = 3,6-dichloro-2,5-dihydroxybenzoquinone) and evaluate the angular dependence of its magnetic properties. Oriented-crystal magnetization measurements reveal strong uniaxial anisotropy, where the easy axis is aligned with the crystallographic c axis. While the spin carriers of this structure are isotropic S = 5/2 FeIII metal centers and S = 1/2 organic linkers, the anisotropy energy of the framework material is comparable to that of reported 2D ferromagnets. Density functional theory calculations indicate that the observed magnetocrystalline anisotropy arises from ligand-to-metal charge transfer that enhances the magnetic anisotropy of the otherwise-isotropic Fe centers, suggesting that metal-ligand covalency can be utilized as a general additive for the development of 2D magnets. These results show the possibility for (NMe4)2[Fe2L3] to retain magnetic order down to the 2D monolayer limit. In addition, the combination of large magnetic anisotropy and semiconducting character in (NMe4)2[Fe2L3] highlights its potential as a new 2D magnetic semiconductor.},
doi = {10.1021/acs.chemmater.1c02670},
journal = {Chemistry of Materials},
number = 22,
volume = 33,
place = {United States},
year = {Tue Nov 02 00:00:00 EDT 2021},
month = {Tue Nov 02 00:00:00 EDT 2021}
}
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