Above-room Curie temperature and barrier-layer-dependent tunneling magnetoresistance in 1T-CrO2 monolayer based magnetic tunnel junctions

van der Waals (vdW) heterostructures based on two-dimensional (2D) ferromagnetic materials hold great potential applications in spintronics. Using the density functional theory (DFT) method and first-principles quantum transport simulation, we studied the structures, magnetic properties and spin-resolved transport of 1T-CrO2 monolayer (ML) based vdW magnetic tunnel junctions (MTJs). Owing to a high Curie temperature (TC) of 392 K and a moderate magnetic anisotropy energy (MAE) of 94 μeV of the ferromagnetic 1T-CrO2 monolayer, Cu(111)|CrO2|nML-Gr|CrO2|Cu(111) MTJs were built. Our results reveal that their tunneling magnetoresistance (TMR) ratios are dependent on the number of Gr barrier layers within a working bias voltage of 1 V. For the thin barrier layers (n = 1-2), the maintained TMR ratios can reach a giant value of about 1 × 104%, while there appears a decreasing trend with the increasing bias voltage for thick Gr layers (n = 3-5). The barrier-layer-dependent phenomenon is attributed to the decreasing transmission magnitude with increasing bias voltage in a parallel configuration (PC), which is as small as that in an anti-parallel configuration (APC) eventually. Our results would provide some guidance for future experimental fabrications of these 2D materials based MTJs.