Interlayer engineering of Fe 3 GeTe 2 : From 3D superlattice to 2D monolayer

Author:

Wu Yecun123ORCID,Wang Bai Yang13,Yu Yijun4,Li Yanbin5,Ribeiro Henrique B.6,Wang Jierong4,Xu Rong5,Liu Yunzhi5,Ye Yusheng5ORCID,Zhou Jiawei5,Ke Feng7,Harbola Varun3,Heinz Tony F.46,Hwang Harold Y.14,Cui Yi15

Affiliation:

1. Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA 94025

2. Department of Electrical Engineering, Stanford University, Stanford, CA 94305

3. Department of Physics, Stanford University, Stanford, CA 94305

4. Department of Applied Physics, Stanford University, Stanford, CA 94305

5. Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305

6. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA 94025

7. Department of Geological Science, Stanford University, Stanford, CA 94305

Abstract

The discoveries of ferromagnetism down to the atomically thin limit in van der Waals (vdW) crystals by mechanical exfoliation have enriched the family of magnetic thin films [C. Gong et al., Nature 546 , 265–269 (2017) and B. Huang et al., Nature 546 , 270–273 (2017)]. However, compared to the study of traditional magnetic thin films by physical deposition methods, the toolbox of the vdW crystals based on mechanical exfoliation and transfer suffers from low yield and ambient corrosion problem and now is facing new challenges to study magnetism. For example, the formation of magnetic superlattice is difficult in vdW crystals, which limits the study of the interlayer interaction in vdW crystals [M. Gibertini, M. Koperski, A. F. Morpurgo, K. S. Novoselov, Nat. Nanotechnol. 14 , 408–419 (2019)]. Here, we report a strategy of interlayer engineering of the magnetic vdW crystal Fe 3 GeTe 2 (FGT) by intercalating quaternary ammonium cations into the vdW spacing. Both three-dimensional (3D) vdW superlattice and two-dimensional (2D) vdW monolayer can be formed by using this method based on the amount of intercalant. On the one hand, the FGT superlattice shows a strong 3D critical behavior with a decreased coercivity and increased domain wall size, attributed to the co-engineering of the anisotropy, exchange interaction, and electron doping by intercalation. On the other hand, the 2D vdW few layers obtained by over-intercalation are capped with organic molecules from the bulk crystal, which not only enhances the ferromagnetic transition temperature ( T C ), but also substantially protects the thin samples from degradation, thus allowing the preparation of large-scale FGT ink in ambient environment.

Funder

U.S. Department of Energy

National Science Foundation

Publisher

Proceedings of the National Academy of Sciences

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