Abstract
This work addresses a significant challenge in engineered molecular systems regarding both understanding and controlling the stability of molecule/nanoparticle nanostructures under ambient exposure. Results deal specifically with molecular electronic junctions, where electronic contacts and transport are known to be sensitive to sample history and ambient exposure. We demonstrate that low-temperature atomic layer deposition can gently encapsulate and stabilize molecular electronic junctions, making it feasible to handle and transport junctions in air for many days with minimal change in electronic conduction. These findings indicate the potential for long-term stability of advanced synthetic nanoparticle/molecule nanoconstructs. For this study, conductivity through nanoparticle/molecule/nanoparticle junctions is analyzed and found to be consistent with nonresonant charge tunneling through a single or a small number of oligomeric phenylene ethynylene molecules in the electrical junction. The conductivity was stable in vacuum and inert gas, but under ambient exposure, the current initially decreased, then increased rapidly, followed by a slower rise, reaching a value exceeding 10 times larger than initially measured. After encapsulating functional devices using atomic layer deposition of aluminum oxide thin films at 30−50 °C, the junction showed conductance similar to the precoated values, and the current remained unchanged after more than 15 days under ambient exposure. The presence of the molecule junction after encapsulation was confirmed by the observed transition to Fowler−Nordheim tunneling and analysis of junction breakdown at high fields. The high conformality, precise thickness control, and low-temperature compatibility of the atomic layer deposition method make it uniquely qualified to stabilize and protect molecular junctions and systems.
Published Version
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