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Hard Ferromagnetism Down to the Thinnest Limit of Iron-Intercalated Tantalum Disulfide

Husremović, Samra and Groschner, Catherine K. and Inzani, Katherine and Craig, Isaac M. and Bustillo, Karen C. and Ercius, Peter and Kazmierczak, Nathanael P. and Syndikus, Jacob and Van Winkle, Madeline and Aloni, Shaul and Taniguchi, Takashi and Watanabe, Kenji and Griffin, Sinéad M. and Bediako, D. Kwabena (2022) Hard Ferromagnetism Down to the Thinnest Limit of Iron-Intercalated Tantalum Disulfide. Journal of the American Chemical Society, 144 (27). pp. 12167-12176. ISSN 0002-7863. doi:10.1021/jacs.2c02885.

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Two-dimensional (2D) magnetic crystals hold promise for miniaturized and ultralow power electronic devices that exploit spin manipulation. In these materials, large, controllable magnetocrystalline anisotropy (MCA) is a prerequisite for the stabilization and manipulation of long-range magnetic order. In known 2D magnetic crystals, relatively weak MCA typically results in soft ferromagnetism. Here, we demonstrate that ferromagnetic order persists down to the thinnest limit of FeₓTaS₂ (Fe-intercalated bilayer 2H-TaS b) with giant coercivities up to 3 T. We prepare Fe-intercalated TaS₂ by chemical intercalation of van der Waals-layered 2H-TaS₂ crystals and perform variable-temperature transport, transmission electron microscopy, and confocal Raman spectroscopy measurements to shed new light on the coupled effects of dimensionality, degree of intercalation, and intercalant order/disorder on the hard ferromagnetic behavior of FeₓTaS₂. More generally, we show that chemical intercalation gives access to a rich synthetic parameter space for low-dimensional magnets, in which magnetic properties can be tailored by the choice of the host material and intercalant identity/amount, in addition to the manifold distinctive degrees of freedom available in atomically thin, van der Waals crystals.

Item Type:Article
Related URLs:
URLURL TypeDescription
Husremović, Samra0000-0002-4741-3780
Groschner, Catherine K.0000-0001-9996-1124
Inzani, Katherine0000-0002-3117-3188
Bustillo, Karen C.0000-0002-2096-6078
Ercius, Peter0000-0002-6762-9976
Kazmierczak, Nathanael P.0000-0002-7822-6769
Syndikus, Jacob0000-0003-4362-4035
Van Winkle, Madeline0000-0001-5772-2723
Aloni, Shaul0000-0002-7561-4336
Taniguchi, Takashi0000-0002-1467-3105
Watanabe, Kenji0000-0003-3701-8119
Griffin, Sinéad M.0000-0002-9943-4866
Bediako, D. Kwabena0000-0003-0064-9814
Additional Information:© 2022 American Chemical Society. Received 16 March 2022. Published online 22 June 2022. Published in issue 13 July 2022. The authors thank Oscar Gonzalez, Zhizhi Kong, Lilia Xie, and Steven Zeltmann for helpful discussion. This material is based upon work supported by the Air Force Office of Scientific Research under AFOSR Award no. FA9550-20-1-0007. We would like to thank Gatan, Inc. as well as P. Denes, A. Minor, J. Ciston, C. Ophus, J. Joseph, and Ian Johnson at LBNL, who contributed to the development of the 4D Camera used for STEM-DPC measurements. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract no. DE-AC02-05CH11231 using NERSC award ERCAP0020898 and ERCAP0020897. M.V.W. acknowledges support from a UCB Chancellor’s Fellowship and NSF Graduate Research Fellowship. Instrumentation used in this work was supported by grants from the W.M. Keck Foundation (Award # 993922), the Canadian Institute for Advanced Research (CIFAR–Azrieli Global Scholar, Award # GS21-011), the Gordon and Betty Moore Foundation EPiQS Initiative (Award #10637), and the 3M Foundation through the 3M Non-Tenured Faculty Award (#67507585). N.P.K. acknowledges support from the Hertz Fellowship and from the National Science Foundation Graduate Research Fellowship under grant no. DGE-1745301. Confocal Raman spectroscopy was supported by a DURIP grant through the Office of Naval Research under Award no. N00014-20-1-2599 (D.K.B.). Experimental and theoretical work at the Molecular Foundry, LBNL was supported by the Office of Science, Office of Basic Energy Sciences, the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. Computational studies were carried out using supercomputing resources of the National Energy Research Scientific Computing Center (NERSC) and the TMF clusters managed by the High-Performance Computing Services Group at LBNL. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan, grant number JPMXP0112101001, JSPS KAKENHI grant number JP20H00354, and the CREST (JPMJCR15F3), JST. The authors declare no competing financial interest.
Funding AgencyGrant Number
Air Force Office of Scientific Research (AFOSR)FA9550-20-1-0007
Department of Energy (DOE)DE-AC02-05CH11231
National Energy Research Scientific Computing CenterERCAP0020898
National Energy Research Scientific Computing CenterERCAP0020897
University of California, BerkeleyUNSPECIFIED
NSF Graduate Research FellowshipDGE-1745301
W. M. Keck Foundation993922
Canadian Institute for Advanced Research (CIFAR)GS21-011
Gordon and Betty Moore Foundation10637
Office of Naval Research (ONR)N00014-20-1-2599
Ministry of Education, Culture, Sports, Science and Technology (MEXT)JPMXP0112101001
Japan Society for the Promotion of Science (JSPS)JP20H00354
Japan Science and Technology AgencyJPMJCR15F3
Subject Keywords:Crystals, Intercalation, Lattices, Magnetic properties, Phase transitions
Issue or Number:27
Record Number:CaltechAUTHORS:20220729-722098000
Persistent URL:
Official Citation:Hard Ferromagnetism Down to the Thinnest Limit of Iron-Intercalated Tantalum Disulfide Samra Husremović, Catherine K. Groschner, Katherine Inzani, Isaac M. Craig, Karen C. Bustillo, Peter Ercius, Nathanael P. Kazmierczak, Jacob Syndikus, Madeline Van Winkle, Shaul Aloni, Takashi Taniguchi, Kenji Watanabe, Sinéad M. Griffin, and D. Kwabena Bediako Journal of the American Chemical Society 2022 144 (27), 12167-12176 DOI: 10.1021/jacs.2c02885
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:115963
Deposited By: George Porter
Deposited On:01 Aug 2022 15:18
Last Modified:01 Aug 2022 15:18

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