Self-assembled contacts for high-yield molecular devices

With their atomic precision and synthetically tailorable properties, molecules offer new possibilities for emerging computing, sensing, optical and quantum technologies. However, the scalable, damage-free integration of molecules into active devices with atomic-scale control remains a critical challenge due to incompatibility with existing top-down fabrication processes. Here we introduce self-assembled contacts, a strategy in which device structures are first fabricated using standard semiconductor manufacturing processes and subsequently transformed through engineered surface interactions to form self-aligned, pristine interfaces with molecules. We validate this approach by fabricating over 1,000 electrically active metal-molecule-metal devices with yields of up to 99% and stable operation over 10⁵ measurement cycles, even for molecular layers thinner than 1 nm. In situ Raman measurements verified the preservation of molecular integrity. Beyond individual devices, the platform supports system-level integration, which we demonstrate through vector-matrix multiplication, a fundamental operation in neuromorphic computing, implemented in a crossbar array of self-rectified molecular memory devices. Our results establish self-assembled contacts as a scalable platform for integrating molecular functionalities into devices, bridging self-assembly and top-down manufacturing.