<p>Achieving continuous, uniform, and large-area monolayers of polymer-grafted nanoparticles (PGNPs) remains challenging, particularly for those bearing weak polyelectrolyte ligands, where electrostatic interactions often cause nonuniform aggregation and discontinuities. Here, we report a facile and efficient liquid/liquid interfacial assembly strategy to fabricate centimeter-scale, continuous monolayers of poly(2-vinylpyridine)-grafted gold nanoparticles (Au@P2VP). By precisely regulating the pH and ionic strength of the aqueous subphase, the protonation degree of P2VP ligands and the interparticle electrostatic interactions were tuned to modulate the interfacial tension and suppress coffee-ring formation, leading to the formation of uniform Au@P2VP monolayers. The resulting films were successfully transferred onto n-type silicon substrates as floating-gate layers for organic field-effect transistor memory devices. Compared with neat P2VP electret layers, the incorporation of Au nanoparticles provided additional charge-trapping sites and improved film continuity, yielding a broad memory window of 40 V, an on/off drain current ratio above 5 × 10<sup>2</sup>, and stable retention exceeding 10<sup>4</sup> s. This study presents a general approach to manipulate weak polyelectrolyte interactions at liquid interfaces for the scalable fabrication of PGNP monolayers and demonstrates their great potential in high-performance nano-floating-gate memories.</p>

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Large-scale polymer-grafted nanoparticle monolayers toward high-performance floating-gate memories

  • Simeng Liu,
  • Mengao Lei,
  • Hao Yu,
  • Yonghao Yang,
  • Yinhan Xu,
  • Wen Li,
  • Mingdong Yi,
  • Jiangping Xu,
  • Jintao Zhu

摘要

Achieving continuous, uniform, and large-area monolayers of polymer-grafted nanoparticles (PGNPs) remains challenging, particularly for those bearing weak polyelectrolyte ligands, where electrostatic interactions often cause nonuniform aggregation and discontinuities. Here, we report a facile and efficient liquid/liquid interfacial assembly strategy to fabricate centimeter-scale, continuous monolayers of poly(2-vinylpyridine)-grafted gold nanoparticles (Au@P2VP). By precisely regulating the pH and ionic strength of the aqueous subphase, the protonation degree of P2VP ligands and the interparticle electrostatic interactions were tuned to modulate the interfacial tension and suppress coffee-ring formation, leading to the formation of uniform Au@P2VP monolayers. The resulting films were successfully transferred onto n-type silicon substrates as floating-gate layers for organic field-effect transistor memory devices. Compared with neat P2VP electret layers, the incorporation of Au nanoparticles provided additional charge-trapping sites and improved film continuity, yielding a broad memory window of 40 V, an on/off drain current ratio above 5 × 102, and stable retention exceeding 104 s. This study presents a general approach to manipulate weak polyelectrolyte interactions at liquid interfaces for the scalable fabrication of PGNP monolayers and demonstrates their great potential in high-performance nano-floating-gate memories.