Two-Dimensional Conductive Metal-Organic Framework Reinforced Spinterface in Organic Spin Valves

Interface engineering in device fabrication is a significant but complicated issue. Although great successes have been achieved by conventional physical in situ or ex situ methods, it still suffers from complicated procedures. In this work, we present a facile method for fabricating phthalocyanine (Pc) based two-dimensional conductive metal-organic framework (MOF) films. Based on PcM-Cu (M = Ni, Cu, H2) MOF films, spin valves with a vertical configuration of La0.67Sr0.33MnO3/PcM-Cu MOFs/Co were constructed successfully, and exhibited notably high negative magnetoresistance (MR) up to -22% at 50 K. The penetrated Co atoms coordinated with the dehydrogenated hydroxy groups in the MOFs resulting in an antiferromagnetic layer of the PcM-Cu-Co hybrid structure. Interestingly, a significant exchange bias effect was demonstrated at the PcM-Cu MOF/Co interface, beneficial for the MR behavior. Thus, our present study provides new insights into developing high-performance organic spin valves via de novo molecular design.