Soft lithography techniques using elastomeric molds have attracted significant interest from researchers during the past two decades.[1–3] Various examples have been presented including microcontact printing, replica molding, solventassisted micromolding, capillary force lithography, micro/nanotransfer molding, micromolding in capillaries, and decal transfer lithography.[1–10] The advantages of these techniques include simplicity, versatility, moderate resolution, low cost, and high throughput, which provide opportunities to readily fabricate various devices such as transistors, sensors, microfluidic devices, and so on.[10] Among these methods, nanotransfer printing (nTP) has shown great potential for conveniently generating various functional inorganic nanostructures such as gold, TiO 2, SnO 2, ZnO, and so on.[11–14] The achievement of a sub-10 nm resolution using soft lithography adds an important technological significance in that well-aligned quantum wires with unusual properties that result from the quantum size effect can be produced for applications in printed electronic devices with significantly enhanced performances. However, in previous approaches, the minimum possible dimension of nTP has been limited to approximately 50 nm primarily due to the collapse and merging of the molds during transfer printing, resulting from the low modulus of elastomers.[10] Although a relatively improved resolution of 20 nm was reported through the adjustment of the modulus and surface energy of elastomers,[15] the partial deformation and degraded quality of their replicated patterns still remain as issues. The resolution and throughput of the lithographic techniques required for the patterning of the original silicon masters, which are used to prepare elastomeric molds, are also critical challenges. The minimum possible feature size that can be defined by conventional photolithography is usually significantly larger than 10 nm. As an alternative, electron beam lithography (EBL) can be considered, but the very low throughput of EBL prevents it from scaling up the process; furthermore, the best resolutions of the elastomeric molds fabricated by EBL have not yet been demonstrated near the 10 nm range.

There have been approaches that enhance the resolution of nanoimprint lithography (NIL) based on hard molds using block copolymer (BCP) self-assembly.[16, 17] This directed selfassembly (DSA) can produce useful nanostructures by controlling the position and orientation of the self-assembled patterns of the BCPs using guiding templates defined by lithographic techniques.[18–23] The microphase-separation of two mutually incompatible blocks in a BCP leads to the formation of ordered arrays of sub-30 nm features such as spherical, cylindrical or lamellar structures depending on the volumetric composition of the individual component.[24, 25] DSA has shown promising potential to complement advanced optical lithography techniques by enhancing their resolution a few to tens of times.[23, 26–29] Although the DSA of BCPs has provided opportunities to fabricate nanoscale devices such as transistors, memory devices, and sensors,[30–34] it usually demands topographic or chemical guiding templates or a proper surface functionalization to control the position and orientation of the self-assembly patterns or for facilitating the self-assembly process.[21, 22, 31–34] Such requirements can seriously restrict the range of applications because some types of substrates and thin films are vulnerable to attacks from solvents that are used to coat and develop photoresists and apply surface modifications. Here, we report how a method of the synergic combination of …