Efficient Integration of Self-Assembled Organic Monolayer Tunnel Barriers in Large-Area Pinhole-Free Magnetic Tunnel Junctions

Magneto-transport properties in hybrid magnetic tunnel junctions (MTJs) integrating Self-Assembled Monolayers (SAMs) as tunnel barriers are critically influenced by spinterface effects, which arise from the electronic properties at ferromagnet (FM)/SAM interfaces. Understanding the mechanisms governing spinterface formation in well-controlled model systems is essential for the rational design of efficient molecular spintronic devices. However, the fabrication of FM/SAM/FM systems remains a significant challenge due to the difficulty in preventing electrical shorts through the SAM tunnel barrier during top FM electrode deposition. In this study, we address these challenges by developing model hybrid MTJs incorporating alkanethiol SAM tunnel barriers grafted under ultrahigh vacuum conditions onto single-crystalline Fe(001) bottom electrodes. A soft-landing deposition method is used for the deposition of a top Co FM electrode. The deposition process and the electronic properties of the formed FM/SAM interfaces are first studied by spatially integrated X-ray Photoelectron Spectroscopy (XPS). Furthermore, Ballistic Electron Emission Microscopy (BEEM) and spectroscopy are used to investigate the lateral homogeneity of the organic barrier. Optimal soft-landing deposition conditions allow the preparation of homogeneous Co/SAM interfaces with no evidence of metal diffusion through the SAM at the nanoscale. These observations are further confirmed at the micron scale by the high-yield patterning of large-area (5 × 5 μm 2 ) MTJs presenting fingerprints of electron tunneling through the SAM. These findings provide critical insights into the fabrication and optimization of molecular spintronic devices, paving the way for advancements in hybrid MTJ technology.