A Centimeter-Scale Inorganic Nanoparticle Superlattice Monolayer with Non-Close-Packing and its High Performance in Memory Devices

Due to the near-field coupling effect, non-close-packed nanoparticle (NP) assemblies with tunable interparticle distance (d) attract great attention and show huge potential applications in various functional devices, e.g., organic nano-floating-gate memory (NFGM) devices. Unfortunately, the fabrication of device-scale non-close-packed 2D NPs material still remains a challenge, limiting its practical applications. Here, a facile yet robust “rapid liquid–liquid interface assembly” strategy is reported to generate a non-close-packed AuNP superlattice monolayer (SM) on a centimeter scale for high-performance pentacene-based NFGM. The d and hence the surface plasmon resonance spectra of SM can be tailored by adjusting the molecular weight of tethered polymers. Precise control over the d value allows the successful fabrication of photosensitive NFGM devices with highly tunable performances from short-term memory to nonvolatile data storage. The best performing nonvolatile memory device shows remarkable 8-level (3-bit) storage and a memory ratio over 10⁵ even after 10 years compared with traditional devices with a AuNP amorphous monolayer. This work provides a new opportunity to obtain large area 2D NPs materials with non-close-packed structure, which is significantly meaningful to microelectronic, photovoltaics devices, and biochemical sensors.