Surface‐Selective Nucleation of Polymeric Resists for Bottom‐Up Nanofabrication

Bottom-up micro/nanofabrication complements photolithography in multilayer, 3D, and cost-effective manufacturing, but lacks resist patterning technology with photoresist-level reproducibility, processability, and universality. Here, we explore a surface-selective nucleation (SSN) effect to derive polymeric resist patterns with nanoscale resolution, inherent 3D compatibility, low defect density, clean lift-off, and broad applicability across fabrication platforms. The SSN phenomenon is achieved through solution-phase polymerization of dual-ended acrylic monomers on prepatterned substrates and surface-mediated creation of area-dependent nucleation barriers using adsorption inhibitors and chain terminators, which synergistically modulate surface and bulk free energy of nucleation, respectively. The resulting resist forms a coherent resin film physically adhered to the substrate, while featuring tunable thickness (13-150 nm) and minimal surface roughness (0.91 nm). This method delivers 15 nm linewidth patterning with 99.97% coverage across wafer-scale arrays within 10 s and demonstrates high compatibility with mainstream thin-film deposition techniques (e.g., e-beam evaporation, sputtering, and atomic layer deposition).