- Chen, Xiang;
- Shao, Yu-Tsun;
- Chen, Rui;
- Susarla, Sandhya;
- Hogan, Tom;
- He, Yu;
- Zhang, Hongrui;
- Wang, Siqi;
- Yao, Jie;
- Ercius, Peter;
- Muller, David A;
- Ramesh, Ramamoorthy;
- Birgeneau, Robert J
The existence of long-range magnetic order in low-dimensional magnetic systems, such as the quasi-two-dimensional van der Waals (vdW) magnets, has attracted intensive studies of new physical phenomena. The vdW Fe_{N}GeTe_{2} (N=3, 4, 5; FGT) family is exceptional, owing to its vast tunability of magnetic properties. In particular, a ferromagnetic ordering temperature (T_{C}) above room temperature at N=5 (F5GT) is observed. Here, our study shows that, by nickel (Ni) substitution of iron in F5GT, a record high T_{C}=478(6) K is achieved. Importantly, pervasive, beyond room-temperature ferromagnetism exists in almost the entire doping range of the phase diagram of Ni-F5GT. We argue that this striking observation in Ni-F5GT can be possibly due to several contributing factors, including increased 3D magnetic couplings due to the structural alterations.