Journal Home > Volume 15 , Issue 1
Nano Research 2022, 15(1): 457-464 https://doi.org/10.1007/s12274-021-3502-0
Research Article | Issue | Published: 01 June 2021

Phase-pure two-dimensional FexGeTe2 magnets with near-room- temperature TC

Show Author's Information Govindan Kutty Rajendran Nair1,§,  Zhaowei Zhang2,§,  Fuchen Hou3,6,§,  Ali Abdelaziem1,4,7,§,  Xiaodong Xu5,  Steve Wu Qing Yang2,  Nan Zhang2,  Weiqi Li5,  Chao Zhu1,  Yao Wu1,  Heng Weiling1,  Lixing Kang1,  Teddy Salim1,  Jiadong Zhou1,  Lin Ke2,  Junhao Lin3,6,  Xingji Li5( ),  Weibo Gao2( ),  Zheng Liu1,8,9( )
School of Material Science and Engineering 50 Nanyang Ave 639798 Singapore
Division of Physics and Applied Physics School of Physical and Mathematical Sciences, Nanyang Technological University21 Nanyang Link 637371 Singapore
Department of Physics, Southern University of Science and Technology Shenzhen 518055 China
Institute of Materials Research and Engineering Agency for Science Technology and Research (A*STAR)2 Fusionopolis Way, Singapore 138634 Singapore
School of Material Science and Engineering School of Physics, Harbin Institute of TechnologyHarbin 150001 China
Shenzhen Key Laboratory of for Advanced Quantum Functional Materials and Devices Southern University of Science and TechnologyShenzhen 518055 China
National Institute of Laser Enhanced Sciences (NILES) Cairo UniversityGiza 12613 Egypt
CINTRA CNRS/NTU/THALES UMI 3288Research Techno Plaza 637553 Singapore
School of Electrical and Electronic Engineering Nanyang Technological University50 Nanyang Ave 639798 Singapore

§ Govindan Kutty Rajendran Nair, Zhaowei Zhang, Fuchen Hou, and Ali Abdelaziem contributed equally to this work.

Keywords:
van der Waals (vdW), terahertz, ferromagnetism, cascaded space confined chemical vapor deposition (CVD), out of plane anisotropy, iron germanium telluride
Topics:
Magnetism
Cite this article:
Nair GKR, Zhang Z, Hou F, et al. Phase-pure two-dimensional FexGeTe2 magnets with near-room- temperature TC. Nano Research, 2022, 15(1): 457-464. https://doi.org/10.1007/s12274-021-3502-0
Download citation
EndNote(RIS)
BibTeX

818

Views

49

Downloads

Citations

21

Crossref

22

WoS

19

Scopus

0

CSCD

Abstract Full text Electronic supplementary material About this article

Two-dimensional (2D) ferromagnets with out-of-plane (OOP) magnetic anisotropy are potential candidates for realizing the next-generation memory devices with ultra-low power consumption and high storage density. However, a scalable approach to synthesize 2D magnets with OOP anisotropy directly on the complimentary metal-oxide semiconductor (CMOS) compatible substrates has not yet been mainly explored, which hinders the practical application of 2D magnets. This work demonstrates a cascaded space confined chemical vapor deposition (CS-CVD) technique to synthesize 2D FexGeTe2 ferromagnets. The weight fraction of iron (Fe) in the precursor controls the phase purity of the as-grown FexGeTe2. As a result, high-quality Fe3GeTe2 and Fe5GeTe2 flakes have been grown selectively using the CS-CVD technique. Curie temperature (TC) of the as-grown FexGeTe2 can be up to ~ 280 K, nearly room temperature. The thickness and temperature-dependent magnetic studies on the Fe5GeTe2 reveal a 2D Ising to 3D XY behavior. Also, Terahertz spectroscopy experiments on Fe5GeTe2 display the highest conductivity among other FexGeTe2 2D magnets. The results of this work indicate a scalable pathway for the direct growth and integration of 2D ternary magnets on CMOS-based substrates to develop spintronic memory devices.


menu
Abstract
Full text
Outline
Electronic supplementary material
About this article

Phase-pure two-dimensional FexGeTe2 magnets with near-room- temperature TC

Show Author's information Govindan Kutty Rajendran Nair1,§, Zhaowei Zhang2,§, Fuchen Hou3,6,§, Ali Abdelaziem1,4,7,§, Xiaodong Xu5, Steve Wu Qing Yang2, Nan Zhang2, Weiqi Li5, Chao Zhu1, Yao Wu1, Heng Weiling1, Lixing Kang1, Teddy Salim1, Jiadong Zhou1, Lin Ke2, Junhao Lin3,6, Xingji Li5( ), Weibo Gao2( ), Zheng Liu1,8,9( )
School of Material Science and Engineering 50 Nanyang Ave 639798 Singapore
Division of Physics and Applied Physics School of Physical and Mathematical Sciences, Nanyang Technological University21 Nanyang Link 637371 Singapore
Department of Physics, Southern University of Science and Technology Shenzhen 518055 China
Institute of Materials Research and Engineering Agency for Science Technology and Research (A*STAR)2 Fusionopolis Way, Singapore 138634 Singapore
School of Material Science and Engineering School of Physics, Harbin Institute of TechnologyHarbin 150001 China
Shenzhen Key Laboratory of for Advanced Quantum Functional Materials and Devices Southern University of Science and TechnologyShenzhen 518055 China
National Institute of Laser Enhanced Sciences (NILES) Cairo UniversityGiza 12613 Egypt
CINTRA CNRS/NTU/THALES UMI 3288Research Techno Plaza 637553 Singapore
School of Electrical and Electronic Engineering Nanyang Technological University50 Nanyang Ave 639798 Singapore

§ Govindan Kutty Rajendran Nair, Zhaowei Zhang, Fuchen Hou, and Ali Abdelaziem contributed equally to this work.

Abstract

Two-dimensional (2D) ferromagnets with out-of-plane (OOP) magnetic anisotropy are potential candidates for realizing the next-generation memory devices with ultra-low power consumption and high storage density. However, a scalable approach to synthesize 2D magnets with OOP anisotropy directly on the complimentary metal-oxide semiconductor (CMOS) compatible substrates has not yet been mainly explored, which hinders the practical application of 2D magnets. This work demonstrates a cascaded space confined chemical vapor deposition (CS-CVD) technique to synthesize 2D FexGeTe2 ferromagnets. The weight fraction of iron (Fe) in the precursor controls the phase purity of the as-grown FexGeTe2. As a result, high-quality Fe3GeTe2 and Fe5GeTe2 flakes have been grown selectively using the CS-CVD technique. Curie temperature (TC) of the as-grown FexGeTe2 can be up to ~ 280 K, nearly room temperature. The thickness and temperature-dependent magnetic studies on the Fe5GeTe2 reveal a 2D Ising to 3D XY behavior. Also, Terahertz spectroscopy experiments on Fe5GeTe2 display the highest conductivity among other FexGeTe2 2D magnets. The results of this work indicate a scalable pathway for the direct growth and integration of 2D ternary magnets on CMOS-based substrates to develop spintronic memory devices.

Keywords: van der Waals (vdW), terahertz, ferromagnetism, cascaded space confined chemical vapor deposition (CVD), out of plane anisotropy, iron germanium telluride

References(41)

1

Huang, B.; Clark, G.; Navarro-Moratalla, E.; Klein, D. R.; Cheng, R.; Seyler, K. L.; Zhong, D.; Schmidgall, E.; McGuire, M. A.; Cobden, D. H. et al. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. Nature 2017, 546, 270–273.
DOI Google Scholar
2

Gong, C.; Li, L.; Li, Z. L.; Ji, H. W.; Stern, A.; Xia, Y.; Cao, T.; Bao, W.; Wang, C. Z.; Wang, Y. et al. Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals. Nature 2017, 546, 265– 269.
DOI Google Scholar
3

O'Hara, D. J.; Zhu, T. C.; Trout, A. H.; Ahmed, A. S.; Luo, Y. K.; Lee, C. H.; Brenner, M. R.; Rajan, S.; Gupta, J. A.; McComb, D. W. et al. Room temperature intrinsic ferromagnetism in epitaxial manganese selenide films in the monolayer limit. Nano Lett. 2018, 18, 3125– 3131.
DOI Google Scholar
4

Bonilla, M.; Kolekar, S.; Ma, Y. J.; Diaz, H. C.; Kalappattil, V.; Das, R.; Eggers, T.; Gutierrez, H. R.; Phan, M. H.; Batzill, M. Strong room- temperature ferromagnetism in VSe2 monolayers on van der Waals substrates. Nat. Nanotechnol. 2018, 13, 289–293.
DOI Google Scholar
5

Fei, Z. Y.; Huang, B.; Malinowski, P.; Wang, W. B.; Song, T. C.; Sanchez, J.; Yao, W.; Xiao, D.; Zhu, X. Y.; May, A. F. et al. Two-dimensional itinerant ferromagnetism in atomically thin Fe3GeTe2. Nat. Mater. 2018, 17, 778–782.
DOI Google Scholar
6

May, A. F.; Ovchinnikov, D.; Zheng, Q.; Hermann, R.; Calder, S.; Huang, B.; Fei, Z. Y.; Liu, Y. H.; Xu, X. D.; McGuire, M. A. Ferromagnetism near room temperature in the cleavable van der Waals crystal Fe5GeTe2. ACS Nano 2019, 13, 4436–4442.
DOI Google Scholar
7

Wu, D.; Zhang, Z.; Li, L.; Zhang, Z. Z.; Zhao, H. B.; Wang, J.; Ma, B.; Jin, Q. Y. Perpendicular magnetic anisotropy and magnetization dynamics in oxidized CoFeAl films. Sci. Rep. 2015, 5, 12352.
DOI Google Scholar
8

Sbiaa, R.; Meng, H.; Piramanayagam, S. N. Materials with perpendicular magnetic anisotropy for magnetic random access memory. Phys. Status Solidi Rapid Res. Lett. 2011, 5, 413–419.
DOI Google Scholar
9

Liu, T.; Cai, J. W.; Sun, L. Large enhanced perpendicular magnetic anisotropy in CoFeB/MgO system with the typical Ta buffer replaced by an Hf layer. AIP Adv. 2012, 2, 032151.
DOI Google Scholar
10

Docherty, C. J.; Parkinson, P.; Joyce, H. J.; Chiu, M. H.; Chen, C. H.; Lee, M. Y.; Li, L. J.; Herz, L. M.; Johnston, M. B. Ultrafast transient terahertz conductivity of monolayer MoS2 and WSe2 grown by chemical vapor deposition. ACS Nano 2014, 8, 11147–11153.
DOI Google Scholar
11

Stahl, J.; Shlaen, E.; Johrendt, D. The van der Waals ferromagnets Fe5–δGeTe2 and Fe5–δ–xNixGeTe2-crystal structure, stacking faults, and magnetic properties. Z. Anorg. Allg. Chem. 2018, 644, 1923–1929.
DOI Google Scholar
12

Yamashita, T.; Hayes, P. Analysis of XPS spectra of Fe2+ and Fe3+ ions in oxide materials. Appl. Surf. Sci. 2008, 254, 2441–2449.
DOI Google Scholar
13

Lloyd-Hughes, J.; Jeon, T. I. A review of the terahertz conductivity of bulk and nano-materials. J. Infrared Millim. Terahertz Waves 2012, 33, 871–925.
DOI Google Scholar
14

Lu, W.; Ling, J. W.; Xiu, F. X.; Sun, D. Terahertz probe of photo­excited carrier dynamics in the Dirac semimetal Cd3As2. Phys. Rev. B 2018, 98, 104310.
DOI Google Scholar
15

McGuire, M. A.; Dixit, H.; Cooper, V. R.; Sales, B. C. Coupling of crystal structure and magnetism in the layered, ferromagnetic insulator CrI3. Chem. Mater. 2015, 27, 612–620.
DOI Google Scholar
16

Siberchicot, B.; Jobic, S.; Carteaux, V.; Gressier, P.; Ouvrard, G. Band structure calculations of ferromagnetic chromium tellurides CrSiTe3 and CrGeTe3. J. Phys. Chem. 1996, 100, 5863–5867.
DOI Google Scholar
17

Seo, J.; Kim, D. Y.; An, E. S.; Kim, K.; Kim, G. Y.; Hwang, S. Y.; Kim, D. W.; Jang, B. G.; Kim, H.; Eom, G. et al. Nearly room temperature ferromagnetism in a magnetic metal-rich van der Waals metal. Sci. Adv. 2020, 6, eaay8912.
DOI Google Scholar
18

Kim, K.; Seo, J.; Lee, E.; Ko, K. T.; Kim, B. S.; Jang, B. G.; Ok, J. M.; Lee, J.; Jo, Y. J.; Kang, W. Large anomalous Hall current induced by topological nodal lines in a ferromagnetic van der Waals semimetal. Nat. Mater. 2018, 17, 794–799.
DOI Google Scholar
19

Matsuda, T.; Kanda, N.; Higo, T.; Armitage, N. P.; Nakatsuji, S.; Matsunaga, R. Room-temperature terahertz anomalous Hall effect in Weyl antiferromagnet Mn3Sn thin films. Nat. Commun. 2020, 11, 909.
DOI Google Scholar
20

Huisman, T. J.; Mikhaylovskiy, R. V.; Telegin, A. V.; Sukhorukov, Y. P.; Granovsky, A. B.; Naumov, S. V.; Rasing, T.; Kimel, A. V. Terahertz magneto-optics in the ferromagnetic semiconductor HgCdCr2Se4. Appl. Phys. Lett. 2015, 106, 132411.
DOI Google Scholar
21

Deng, Y. J.; Yu, Y. J.; Song, Y. C.; Zhang, J. Z.; Wang, N. Z.; Sun, Z. Y.; Yi, Y. F.; Wu, Y. Z.; Wu, S. W.; Zhu, J. Y. et al. Gate-tunable room- temperature ferromagnetism in two-dimensional Fe3GeTe2. Nature 2018, 563, 94–99.
DOI Google Scholar
22

Liu, B. J.; Zou, Y. M.; Zhou, S. M.; Zhang, L.; Wang, Z.; Li, H. X.; Qu, Z.; Zhang, Y. H. Critical behavior of the van der Waals bonded high TC ferromagnet Fe3GeTe2. Sci. Rep. 2017, 7, 6184.
DOI Google Scholar
23

Liu, B. J.; Zou, Y. M.; Zhang, L.; Zhou, S. M.; Wang, Z.; Wang, W. K.; Qu, Z.; Zhang, Y. H. Critical behavior of the quasi-two-dimensional semiconducting ferromagnet CrSiTe3. Sci. Rep. 2016, 6, 33873.
DOI Google Scholar
24

Li, Z. X.; Xia, W.; Su, H.; Yu, Z. H.; Fu, Y. P.; Chen, L. M.; Wang, X.; Yu, N.; Zou, Z. Q.; Guo, Y. F. Magnetic critical behavior of the van der Waals Fe5GeTe2 crystal with near room temperature ferromagnetism. Sci. Rep. 2020, 10, 15345.
DOI Google Scholar
25

Kim, D.; Park, S.; Lee, J.; Yoon, J.; Joo, S.; Kim, T.; Min, K. J.; Park, S. Y.; Kim, C.; Moon, K. W. et al. Antiferromagnetic coupling of van der Waals ferromagnetic Fe3GeTe2. Nanotechnology 2019, 30, 245701.
DOI Google Scholar
26

Yi, J. Y.; Zhuang, H. L.; Zou, Q.; Wu, Z. M.; Cao, G. X.; Tang, S. W.; Calder, S. A.; Kent, P. R. C.; Mandrus, D.; Gai, Z. Competing antiferromagnetism in a quasi-2D itinerant ferromagnet: Fe3GeTe2. 2D Mater. 2016, 4, 011005.
DOI Google Scholar
27

Poulopoulos, P.; Krishnan, R.; Flevaris, N. K. Antiferromagnetic-like coupling evidence in a Pd-Ni multilayer with inverted hysteresis features. J. Magn. Magn. Mater. 1996, 163, 27–31.
DOI Google Scholar
28

Ziese, M.; Vrejoiu, I.; Hesse, D. Inverted hysteresis and giant exchange bias in La0.7Sr0.3MnO3/SrRuO3 superlattices. Appl. Phys. Lett. 2010, 97, 052504.
DOI Google Scholar
29

Geshev, J.; Viegas, A. D. C.; Schmidt, J. E. Unusual remanent magnetization of granular Co/Cu. J. Magn. Magn. Mater. 1999, 196–197, 126–127.
DOI Google Scholar
30

Tokura, Y.; Nagaosa, N. Orbital physics in transition-metal oxides. Science 2000, 288, 462–468.
DOI Google Scholar
31

Rödl, C.; Fuchs, F.; Furthmüller, J.; Bechstedt, F. Quasiparticle band structures of the antiferromagnetic transition-metal oxides MnO, FeO, CoO, and NiO. Phys. Rev. B 2009, 79, 235114.
DOI Google Scholar
32

Zhou, S. S.; Gan, L.; Wang, D. L.; Li, H. Q.; Zhai, T. Y. Space- confined vapor deposition synthesis of two dimensional materials. Nano Res. 2018, 11, 2909–2931.
DOI Google Scholar
33

Yan, C. Y.; Gan, L.; Zhou, X.; Guo, J.; Huang, W. J.; Huang, J. W.; Jin, B.; Xiong, J.; Zhai, T. Y.; Li, Y. R. Space-confined chemical vapor deposition synthesis of ultrathin HfS2 flakes for optoelectronic application. Adv. Funct. Mater. 2017, 27, 1702918.
DOI Google Scholar
34

Tang, L.; Teng, C. J.; Luo, Y. T.; Khan, U.; Pan, H. Y.; Cai, Z. Y.; Zhao, Y.; Liu, B. L.; Cheng, H. M. Confined van der Waals epitaxial growth of two-dimensional large single-crystal In2Se3 for flexible broadband photodetectors. Research 2019, 2019, 2763704.
DOI Google Scholar
35

Kresse, G.; Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 1996, 54, 11169.
DOI Google Scholar
36

Kresse, G.; Furthmüller, J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Comput. Mater. Sci. 1996, 6, 15–50.
DOI Google Scholar
37

Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 1994, 50, 17953.
DOI Google Scholar
38

Kresse, G.; Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 1999, 59, 1758.
DOI Google Scholar
39

Klimeš, J.; Bowler, D. R.; Michaelides, A. Chemical accuracy for the van der Waals density functional. J. Condens. Matter. Phys. 2009, 22, 022201.
DOI Google Scholar
40

Klimeš, J.; Bowler, D. R.; Michaelides, A. Van der Waals density functionals applied to solids. Phys. Rev. B 2011, 83, 195131.
DOI Google Scholar
41

Perdew, J. P.; Burke, K.; Ernzerhof, M. Generalized gradient approximation made simple. Physical Review Letters 1996, 77, 3865.
DOI Google Scholar
File
12274_2021_3502_MOESM1_ESM.pdf (4.3 MB)
Publication history
Copyright
Acknowledgements

Publication history

Received: 21 January 2021
Revised: 20 March 2021
Accepted: 06 April 2021
Published: 01 June 2021
Issue date: January 2022

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

G. K., Z. Z., F. H., and A. L., contributed equally to this work. G. K and Z. L. conceived the research. G. K., W. Y., H. W. synthesized the samples. G. K., A. L., L. K., Z. N., and S. Y. performed the terahertz measurements and analyzed the THz results. F. H. and J. L. carried out STEM studies. Z. Z. and G. W. carried out the RMCD measurements. G. K. and T. S. performed the XPS characterizations. X. X. and X. L. carried out the DFT calculations. All authors helped to analyze data, discussed and interpreted detailed results, and co-wrote the manuscript.

This work was supported from National Research Foundation Singapore programme NRF-CRP22-2019-0007, NRF-CRP22- 2019-0004 and NRF-CRP21-2018-0007. This work was also supported by the Ministry of Education, Singapore, under its AcRF Tier 3 Programme 'Geometrical Quantum Materials' (MOE2018-T3-1-002), AcRF Tier 2 (MOE2019-T2-2-105) and AcRF Tier 1 RG4/17 and RG7/18. We also thank the funding support from National Research foundation (NRF-CRP22- 2019-0004).

Return