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Delocalized carbon-based radical species with unpaired spin, such asphenalenyl (PLY) radical, opened avenues for developing multifunctional organicspintronic devices. Here we develop a novel technique based on athree-dimensional shadow mask and the in-situ deposition to fabricate PLY-,Cu-PLY-, and Zn-PLY-based organic magnetic tunnel junctions (OMTJs) with area3x8 {\mu}m2 and improved morphology. The nonlinear and weaklytemperature-dependent current-voltage (I-V) characteristics in combination withthe low organic barrier height suggest tunneling as the dominant transportmechanism in the structurally and dimensionally optimized OMTJs. Cu-PLY-basedOMTJs, show a significant magnetoresistance up to 14 percent at roomtemperature due to the formation of hybrid states at the metal-moleculeinterfaces called spinterface, which reveals the importance of spin-dependentinterfacial modification in OMTJs design. In particular, Cu-PLY OMTJs shows astable voltage-driven resistive switching response that suggests their use as anew viable and scalable platform for building molecular scale quantummemristors and processors.

Interface-Assisted Room-Temperature Magnetoresistance in Cu-Phenalenyl-based Magnetic Tunnel Junctions