Defect Rectification in High‐Density Patterns through Directed Self‐Assembly of Advanced Block Copolymer Architectures

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The development of high‐density nanoscale patterns is essential for advancing semiconductor devices, data storage media, and various emerging technologies, yet achieving precise control over pattern quality at increasingly smaller dimensions remains a significant challenge. Combining directed self‐assembly (DSA) of block copolymers (BCPs) with high‐resolution photolithography offers a promising approach for precise pattern transfer and potential defect rectification in nanopatterning. Here, how different polymer architectures—linear AB, linear A 1 B 1 A 2 B 2 tetra‐, and comb‐linear BCPs—interact with and rectify common lithographic defects in hexagonally packed cylinder arrays, using coarse‐grained molecular simulations on 2D guide substrates is systematically investigated. The findings reveal that molecular architecture plays a crucial role in achieving both high pattern density and defect tolerance: Linear AB BCPs offer robust defect rectification for most defect types but are sensitive to volume mismatch; linear A 1 B 1 A 2 B 2 tetra‐BCPs enable higher packing densities with tolerance to edge roughness and placement errors; and comb‐linear BCPs support unprecedented density through honeycomb formation while maintaining stable pattern quality across a wide range of guide pattern fractions. This investigation provides insights into strategically engineering polymer architecture to overcome limitations in pattern density and defect tolerance, informing the design of next‐generation nanopatterning materials.