TY - JOUR
T1 - Magnetic properties of intercalated quasi-2D Fe3-xGeTe2 van der Waals magnet
AU - Iturriaga, Hector
AU - Martinez, Luis M.
AU - Mai, Thuc T.
AU - Biacchi, Adam J.
AU - Augustin, Mathias
AU - Hight Walker, Angela R.
AU - Sanad, Mohamed Fathi
AU - Sreenivasan, Sreeprasad T.
AU - Liu, Yu
AU - Santos, Elton J.G.
AU - Petrovic, Cedomir
AU - Singamaneni, Srinivasa R.
N1 - Funding Information:
This material is based upon work supported by the National Science Foundation Graduate Research Fellowship Program under Grant No. 184874.1 Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Science Foundation. S.R.S. and H.I. acknowledge support from the NSF-DMR (Award No. 2105109). S.R.S. acknowledges support from NSF-MRI (Award No. 2018067). E.J.G.S. acknowledges computational resources through CIRRUS Tier-2 HPC Service (ec131 Cirrus Project) at EPCC ( http://www.cirrus.ac.uk ) funded by the University of Edinburgh and EPSRC (EP/P020267/1); ARCHER UK National Supercomputing Service ( http://www.archer.ac.uk ) via Project d429. E.J.G.S. acknowledges the Spanish Ministry of Science’s grant program “Europa-Excelencia” under grant number EUR2020-112238, the EPSRC Open Fellowship (EP/T021578/1), and the Edinburgh-Rice Strategic Collaboration Awards for funding support. Work at Brookhaven National Laboratory was supported by the US Department of Energy, Office of Basic Energy Science, Division of Materials Science and Engineering, under Contract No. DE-SC0012704 (crystal growth). For the purpose of open access, the authors have applied a creative commons attribution (CC BY) licence to any author accepted manuscript version arising. Certain commercial equipment, instruments, or materials are identified in this manuscript in order to specify the experimental procedure adequately. Such identification is not intended to imply recommendation or endorsement by the National Institute of Standards and Technology, nor is it intended to imply that the materials or equipment are necessarily the best available for the purpose.
Funding Information:
This material is based upon work supported by the National Science Foundation Graduate Research Fellowship Program under Grant No. 184874.1 Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Science Foundation. S.R.S. and H.I. acknowledge support from the NSF-DMR (Award No. 2105109). S.R.S. acknowledges support from NSF-MRI (Award No. 2018067). E.J.G.S. acknowledges computational resources through CIRRUS Tier-2 HPC Service (ec131 Cirrus Project) at EPCC (http://www.cirrus.ac.uk) funded by the University of Edinburgh and EPSRC (EP/P020267/1); ARCHER UK National Supercomputing Service (http://www.archer.ac.uk) via Project d429. E.J.G.S. acknowledges the Spanish Ministry of Science’s grant program “Europa-Excelencia” under grant number EUR2020-112238, the EPSRC Open Fellowship (EP/T021578/1), and the Edinburgh-Rice Strategic Collaboration Awards for funding support. Work at Brookhaven National Laboratory was supported by the US Department of Energy, Office of Basic Energy Science, Division of Materials Science and Engineering, under Contract No. DE-SC0012704 (crystal growth). For the purpose of open access, the authors have applied a creative commons attribution (CC BY) licence to any author accepted manuscript version arising. Certain commercial equipment, instruments, or materials are identified in this manuscript in order to specify the experimental procedure adequately. Such identification is not intended to imply recommendation or endorsement by the National Institute of Standards and Technology, nor is it intended to imply that the materials or equipment are necessarily the best available for the purpose.
Publisher Copyright:
© 2023, Springer Nature Limited.
PY - 2023/8/21
Y1 - 2023/8/21
N2 - Among several well-known transition metal-based compounds, cleavable van der Waals (vdW) Fe3-xGeTe2 (FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (TC ~154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the TC 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.
AB - Among several well-known transition metal-based compounds, cleavable van der Waals (vdW) Fe3-xGeTe2 (FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (TC ~154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the TC 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.
KW - Ferromagnetism
KW - Light
KW - Scattering
UR - https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=pure_uoe&SrcAuth=WosAPI&KeyUT=WOS:001052812500002&DestLinkType=FullRecord&DestApp=WOS
U2 - 10.1038/s41699-023-00417-w
DO - 10.1038/s41699-023-00417-w
M3 - Article
SN - 2397-7132
VL - 7
SP - 1
EP - 8
JO - npj 2D Materials and Applications
JF - npj 2D Materials and Applications
IS - 1
M1 - 56
ER -