Robust Giant Magnetoresistance in 2D Van der Waals Molecular Magnetic Tunnel Junctions

The spin transport across a zero-dimensional (0D) single-molecule sandwiched by two-dimensional (2D) van der Waals (vdW) ferromagnetic electrodes may open vast opportunities to create novel mixed-dimensional spintronics devices. However, this remains unexplored yet. Inspired by the recent discovery of 2D intrinsic ferromagnets Fe₃GeTe₂, using first-principles spin transport calculations, we show that single-molecule junctions based on Fe₃GeTe₂ can yield perfect spin filtering and a significant magnetoresistance (MR) of up to ∼6075%. This remarkable MR is more than 2 orders of magnitude higher than the MR obtained for the corresponding junctions with conventional ferromagnetic metals (e.g., Ni, Fe, and Co). We demonstrate the results of two representative examples that are feasible in the experiments: (i) A benzene or (ii) bezenedithiol (BDT) connected either through a scanning tunneling microscope or break-junction setups. We find that the conductance of BDT junctions is more than 10 times larger than that of the benzene junction due to a much stronger hybridization effect at the molecule–metal interfaces. The key mechanism of the perfect spin filtering and large MR in single-molecule junctions is mainly determined by the intrinsic properties of Fe₃GeTe₂ electrodes, while the actual conductance is determined by the hybridization strength of the majority spin channel at the molecule–metal interfaces. It is also predicted that the perfect spin filtering and the remarkably huge MR are highly insensitive to structural variations, interface defects, and stacking orders of the electrodes. Our results provide important insights for expanding molecular spintronics platforms from conventional ferromagnetic metals to new 2D vdw magnets.