Electronic structure, magnetoresistance and spin filtering in graphene|2 monolayer-CrI3(3)|graphene van der Waals magnetic tunnel junctions

In the pursuit of designing van der Waals magnetic tunneling junctions (vdW-MTJs) with two-dimensional (2D) intrinsic magnets, as well as to quantitatively reveal the microscopic nature governing the vertical tunneling pathways beyond the phenomenological descriptions on CrI(3)-based vdW-MTJs, we investigate the structural configuration, electronic structure and spin-polarized quantum transport of graphene|2 monolayer(2ML)-CrI(3)|graphene heterostructure with Ag(111) layers as the electrode, using density functional theory (DFT) and its combination of non-equilibrium Green’s function (DFT-NEGF) methods. The in-plane lattice of CrI(3) layers is found to be stretched when placed on the graphene (Gr) layer, and the layer-stacking does not show any site selectivity. The charge transfer between CrI(3) and Gr layers make the CrI(3) layer lightly electron-doped, and the Gr layer hole-doped. Excitingly, the inter-layer hybridization between graphene and CrI(3) layers render the CrI(3) layer metallic in the majority spin channel, giving rise to an insulator-to-half-metal transition. Due to the metallic/insulator characteristics of the spin-majority/minority channel of the 2ML-CrI(3) barrier in vdW-MTJs, Gr|2ML-CrI(3)|Gr heterostructures exhibit an almost perfect spin filtering effect (SFE) near the zero bias in parallel magnetization, a giant tunneling magnetoresistance (TMR) ratio up to 2 × 10(4)%, and remarkable negative differential resistance (NDR). Our results not only give an explanation for the observed giant TMR in CrI(3)-based MTJs but also show the direct implications of 2D magnets in vdW-heterostructures.