Flexible Crossbar Molecular Devices with Patterned EGaIn Top Electrodes for Integrated All‐Molecule‐Circuit Implementation

Here, a unique crossbar architecture is designed and fabricated, incorporating vertically integrated self‐assembled monolayers in electronic devices. This architecture is used to showcase 100 individual vertical molecular junctions on a single chip with a high yield of working junctions and high device uniformity. The study introduces a transfer approach for patterned liquid‐metal eutectic alloy of gallium and indium top electrodes, enabling the creation of fully flexible molecular devices with electrical functionalities. The devices exhibit excellent charge transport performance, sustain a high rectification ratio (>10 3 ), and stable endurance and retention properties, even when the devices are significantly bent. Furthermore, Boolean logic gates, including OR and AND gates, as well as half‐wave and full‐wave rectifying circuits, are successfully implemented. The unique design of the flexible molecular device represents a significant step in harnessing the potential of molecular devices for high‐density integration and possible molecule‐based computing.