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            Abstract 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 TCremains 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.more » « less
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            Zheng, Wenkai; Xiang, Li; de Quesada, Felipe A.; Augustin, Mathias; Lu, Zhengguang; Wilson, Matthew; Sood, Aditya; Wu, Fengcheng; Shcherbakov, Dmitry; Memaran, Shahriar; et al (, ACS Nano)
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            Chen, Lebing; Chung, Jae-Ho; Stone, Matthew B.; Kolesnikov, Alexander I.; Winn, Barry; Garlea, V. Ovidiu; Abernathy, Douglas L.; Gao, Bin; Augustin, Mathias; Santos, Elton J. G.; et al (, Physical Review X)null (Ed.)
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            Yousaf, Ahmed; Gilliam, Matthew S.; Chang, Shery L.; Augustin, Mathias; Guo, Yuqi; Tahir, Fraaz; Wang, Meng; Schwindt, Alexandra; Chu, Ximo S.; Li, Duo O.; et al (, The Journal of Physical Chemistry C)
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            Wang, Qing Hua; Bedoya-Pinto, Amilcar; Blei, Mark; Dismukes, Avalon H.; Hamo, Assaf; Jenkins, Sarah; Koperski, Maciej; Liu, Yu; Sun, Qi-Chao; Telford, Evan J.; et al (, ACS Nano)
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