In this study we demonstrate that organic radical photopolymerized resins hybridized with inorganic silica nanoparticles improve the mechanical strength of replica mold materials and that organic-inorganic hybridization prolongs mold lifetime independently of mold linewidth during step-and-repeat UV nanoimprinting over 100 cycles. Silica nanoparticles with polymerizable methacryloyl groups (NPMC) were added to 1,10-decanediol dimethacrylate (MC10) and diacrylate (AC10) base monomers to enhance the mechanical properties of the replica molds. Heterogeneous combination of polymerizable groups, such as AC10 and NPMC, maintained a fluidity suitable for molding in UV nanoimprinting, and enabled the preparation of hybrid replica materials with a high inorganic silica content of 56.9 wt% (37.0 vol%). Nanoindentation measurements revealed that the hybrid replica materials with 37.0 vol% silica showed a Young's modulus of 4.4 GPa. Only the 45-nmlinewidth patterns of AC10-based replica molds without NPMC showed line-collapse defects after imprint cycle tests, while the 45- and 100-nm-linewidth shapes of the hybrid resin materials with NPMC remained intact after 128 step-and-repeat imprint cycles and nanoindentation measurements.
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