Magnetic properties of intercalated quasi-2D Fe3-xGeTe2 van der Waals magnet
Source abstract
Abstract
Abstract Among several well-known transition metal-based compounds, cleavable van der Waals (vdW) Fe 3-x GeTe 2 (FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (T C ~154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the T C remains far too low for practical applications, there has been a successful push toward improving it via external driving forces such as pressure, irradiation, and doping. Here we present experimental evidence of a room temperature (RT) ferromagnetic phase induced by the electrochemical intercalation of common tetrabutylammonium cations (TBA+) into quasi-2D FGT. We obtained Curie temperatures as high as 350 K with chemical and physical stability of the intercalated compound. The temperature-dependent Raman measurements, in combination with vdW-corrected ab initio calculations, suggest that charge transfer (electron doping) upon intercalation could lead to the observation of RT ferromagnetism. This work demonstrates that molecular intercalation is a viable route in realizing high-temperature vdW magnets in an inexpensive and reliable manner, and has the potential to be extended to bilayer and few-layer vdW magnets.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: 2D Materials and Applications · Graphene research and applications · Topological Materials and Phenomena
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (39)
Show source-provided references
1. Huang, B. et al. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. Nature 546, 271 (2017).10.1038/nature22391 ↗
2. Gong, C. et al. Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals. Nature 546, 265 (2017).10.1038/nature22060 ↗
3. Jiang, S., Shan, J. & Mak, K. F. Electric-field switching of two-dimensional van der Waals magnets. Nat. Mater. 17, 406 (2018).10.1038/s41563-018-0040-6 ↗
4. Burch, K. S., Mandrus, D. & Park, J.-G. Magnetism in two-dimensional van der Waals materials. Nature 47, 563 (2018).
5. Jenkins, S. et al. Breaking through the Mermin-Wagner limit in 2D van der Waals magnets. Nat. Commun. 13, 6917 (2022).10.1038/s41467-022-34389-0 ↗
6. Cheng Gong, C. & Zhang, X. Two-dimensional magnetic crystals and emergent heterostructure devices. Science 363, 706 (2019).
7. Jiang, S., Li, L., Wang, Z., Mak, K. F. & Shan, J. Controlling magnetism in 2D CrI3 by electrostatic doping. Nat. Nanotechnol. 13, 549–553 (2018).10.1038/s41565-018-0135-x ↗
8. Zhang, X.-X. et al. Gate-tunable spin waves in antiferromagnetic atomic bilayers. Nat. Mater. 19, 838 (2020).10.1038/s41563-020-0713-9 ↗
9. Thiel, L. et al. Probing magnetism in 2D materials at the nanoscale with single-spin microscopy. Science 364, 973–976 (2019).10.1126/science.aav6926 ↗
10. Li, H., Ruan, S. & Zeng, Y.-J. Intrinsic Van Der Waals Magnetic Materials from Bulk to the 2D Limit: New Frontiers of Spintronics. Adv. Mater. 31, 1900065 (2019).10.1002/adma.201900065 ↗
11. Yazyev, O. V. Magnetism in Disordered Graphene and Irradiated Graphite. Phys. Rev. Lett. 101, 037203 (2008).10.1103/PhysRevLett.101.037203 ↗
12. Wang, Y. et al. Room-Temperature Ferromagnetism of Graphene. Nano Lett. 9, 220–224 (2009).10.1021/nl802810g ↗
13. Wu, M., Li, Z., Cao, T. & Louie, S. G. Physical origin of giant excitonic and magnetooptical responses in two-dimensional ferromagnetic insulators. Nat. Commun. 10, 2371 (2019).10.1038/s41467-019-10325-7 ↗
14. Sun, Z. et al. Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3. Nature 572, 497 (2019).10.1038/s41586-019-1445-3 ↗
15. Wang, Q. H. et al. The Magnetic Genome of Two-Dimensional van der Waals Materials. ACS Nano 16, 6960–7079 (2022).10.1021/acsnano.1c09150 ↗
16. Padmanabhan, P. et al. Coherent Helicity-Dependent Spin-Phonon Oscillations in the Ferromagnetic van der Waals Crystal CrI3. Nat. Commun. 13, 4473 (2022).10.1038/s41467-022-31786-3 ↗
17. Singamaneni, S. R. et al. Light Induced Electron Spin Resonance Properties of van der Waals CrX3 (X = Cl, I) Crystals. Appl. Phys. Lett. 117, 082406 (2020).10.1063/5.0010888 ↗
18. Martinez, L. M. et al. Enhanced magnetization in proton irradiated Mn3Si2Te6 van der Waals crystals. Appl. Phys. Lett. 116, 172404 (2020).10.1063/5.0002168 ↗
19. Olmos, R. et al. Critical phenomena of the layered ferrimagnet Mn3Si2Te6 following proton irradiation. J. Appl. Phys. 130, 013902 (2021).10.1063/5.0056387 ↗
20. Olmos, R. et al. Pressure-induced magnetic properties of quasi-2D Cr2Si2Te6 and Mn3Si2Te6. J. Phys. Chem. C 127, 10324–10331 (2023).10.1021/acs.jpcc.3c01091 ↗
21. Liu, Y., Li, J., Tao, J., Zhu, Y. & Petrovic, C. Anisotropic magnetocaloric effect in Fe3-xGeTe2. Sci. Rep. 9, 13233 (2019).10.1038/s41598-019-49654-4 ↗
22. Milosavljević, A. et al. Lattice dynamics and phase transitions in Fe3-x GeTe2. Phys. Rev. B 99, 214304 (2019).10.1103/PhysRevB.99.214304 ↗
23. May, A. F., Calder, S., Cantoni, C., Cao, H. & McGuire, M. A. Magnetic structure and phase stability of the van der Waals bonded ferromagnet Fe3-xGeTe2. Phys. Rev. B 93, 014411 (2016).10.1103/PhysRevB.93.014411 ↗
24. Weber, D., Trout, A. H., McComb, D. W. & Goldberger, J. E. Decomposition-Induced Room-Temperature Magnetism of the Na-Intercalated Layered Ferromagnet Fe3-xGeTe2. Nano Lett. 19, 5031–5035 (2019).10.1021/acs.nanolett.9b01287 ↗
25. Wang, N. et al. Transition from Ferromagnetic Semiconductor to Ferromagnetic Metal with Enhanced Curie Temperature in Cr2Ge2Te6 via Organic Ion Intercalation. J. Am. Chem. Soc. 141, 17166–17173 (2019).10.1021/jacs.9b06929 ↗
26. Bennett, L. H. & Della Torre, E. Analysis of wasp-waist hysteresis loops. J. Appl. Phys. 97, 10E502 (2005).10.1063/1.1846171 ↗
27. Kong, X., Berlijn, T. & Liang, L. Thickness and Spin Dependence of Raman Modes in Magnetic Layered Fe3GeTe2. Adv. Electron. Mater. 7, 2001159 (2021).10.1002/aelm.202001159 ↗
28. Casto, L. D. et al. Strong spin-lattice coupling in CrSiTe3. APL Mater. 3, 041515 (2015).10.1063/1.4914134 ↗
29. Deng, Y. et al. Gate-tunable room-temperature ferromagnetism in two-dimensional Fe3GeTe2. Nature 563, 94–99 (2018).10.1038/s41586-018-0626-9 ↗
30. Fleury, P. A. & Loudon, R. Scattering of Light by One- and Two- Magnon Excitations. Phys. Rev. 166, 514 (1968).10.1103/PhysRev.166.514 ↗
31. Fleury, P. A., Porto, S. P. S., Cheesman, L. E. & Guggenheim, H. J. Light Scattering by Spin Waves in FeF2. Phys. Rev. Lett. 17, 84 (1966).10.1103/PhysRevLett.17.84 ↗
32. Weber, M. C. et al. Emergent spin-phonon coupling through cross-talk of two magnetic sublattices. Nat. Commun. 13, 443 (2022).10.1038/s41467-021-27267-8 ↗
33. Jang, S. W. et al. Origin of ferromagnetism and the effect of doping on Fe3GeTe2. Nanoscale 12, 13501–13506 (2020).10.1039/C9NR10171C ↗
34. Huang, X. et al. Li-ion intercalation enhanced ferromagnetism in van der Waals Fe3GeTe2 bilayer. Appl. Phys. Lett. 119, 012405 (2021).10.1063/5.0051882 ↗
35. Shen, Z.-X., Bo, X., Cao, K., Wan, X. & He, L. Magnetic ground state and electron-doping tuning of Curie temperature in Fe3GeTe2: First-principles studies. Phys. Rev. B 103, 085102 (2021).10.1103/PhysRevB.103.085102 ↗
36. Tan, C. et al. Hard magnetic properties in nanoflake van der Waals Fe3GeTe2. Nat. Commun. 9, 1554 (2018).10.1038/s41467-018-04018-w ↗
37. Liu, S. et al. Wafer-scale two-dimensional ferromagnetic Fe3GeTe2 thin films grown by molecular beam epitaxy. Npj 2D Mater. Appl. 1, 1–7 (2017).10.1038/s41699-017-0006-6 ↗
38. Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. J. Phys. Rev. B 54, 11169 (1996).10.1103/PhysRevB.54.11169 ↗
39. Grimme, S., Antony, J., Ehrlich, S. & Krieg, H. J. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J. Chem. Phys. 132, 154104 (2010).10.1063/1.3382344 ↗