E. Georgopoulou-Kotsaki, *ab   P. Pappas, a   A. Lintzeris, ac   P. Tsipas,a   S. Fragkos, ad   A. Markou,e   C. Felser,e   E. Longo, f   M. Fanciulli, g   R. Mantovan, f   F. Mahfouzi,h   N. Kioussis h  and  A. Dimoulasa  

Nanoscale, 2023,15, 2223-2233, DOI https://doi.org/10.1039/D2NR04820E

Two-dimensional (2D) van der Waals (vdW) ferromagnetic metals FexGeTe2 with x = 3–5 have raised significant interest in the scientific community. Fe5GeTe2 shows prospects for spintronic applications since the Curie temperature Tc has been reported near or higher than 300 K. In the present work, epitaxial Fe5−δGeTe2 (FGT) heterostructures were grown by Molecular Beam Epitaxy (MBE) on insulating crystalline substrates. The FGT films were combined with Bi2Te3 topological insulator (TI) aiming to investigate the possible beneficial effect of the TI on the magnetic properties of FGT. FGT/Bi2Te3 films were compared to FGT capped only with AlOx to prevent oxidation. SQUID and MOKE measurements revealed that the growth of Bi2Te3 TI on FGT films significantly enhances the saturation magnetization of FGT as well as the Tc well above room temperature (RT) reaching record values of 570 K. First-principles calculations predict a shift of the Fermi level and an associated enhancement of the majority spin (primarily) as well as the total density of states at the Fermi level suggesting that effective doping of FGT from Bi2Te3 could explain the enhancement of ferromagnetism in FGT. It is also predicted that strain induced stabilization of a high magnetic moment phase in FGT/Bi2Te3 could be an alternative explanation of magnetization and Tc enhancement. Ferromagnetic resonance measurements evidence an enhanced broadening in the FGT/Bi2Te3 heterostructure when compared to FGT. We obtain a large spin mixing conductance of g↑↓eff = 4.4 × 1020 m−2, which demonstrates the great potential of FGT/Bi2Te3 systems for spin-charge conversion applications at room temperature.

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DOI https://doi.org/10.1039/D2NR04820E