We report on the role of intrinsic ͑adhesion force and wettability͒ and extrinsic ͑temperature and pressure͒ conditions to fabricate dense nanoscale patterns in detachment nanolithography. A phase diagram is constructed by using a rigiflex polymeric mold, an organic film, and silicon or gold substrate. Operating conditions in terms of surface tensions and processing parameters are discussed along with comparison of the minimum resolution with a simple theory. © 2008 American Institute of Physics. ͓DOI: 10.1063/1.2937143͔ Detachment nanolithography is a reverse process of additive transfer methods 1 and provides an alternative route to the fabrication of nanoscale patterns in a simple, one-step manner. A number of detachment-based patterning methods have been introduced with different mold ͑polymer, silicon͒ and film materials ͑metal, polymer, or organic layer͒.2-5 A key operating condition is a reasonable difference in adhesive forces between the mold/film interface ͑W 12 ͒ and the film/substrate interface ͑W 23 ͒, i.e., W 12 Ͼ W 23 . Despite extensive works in this field, the role of film wettability and process parameters as well as the interplay between them has not been well addressed. In this letter, we report on the effects of thermodynamic ͑adhesive forces and wettability͒ and process conditions ͑temperature and pressure͒ to realize dense nanoscale patterns in a typical experimental setup of detachment nanolithography.For experiments, a nanoscale silicon master having 70 nm line-and-space patterns ͑150 nm height, number of lines= 36 per repeating unit͒ was used. The detailed geometry is shown in Fig. 1. A rigiflex polymeric mold of ultraviolet curable polyurethane acrylate ͑PUA͒ was replicated from this silicon master, which was used to detach nanoscale patterns from an underlying layer of 4 , 4Ј-bis͓N-1-napthyl-N-phenyl-amino͔biphenyl ͑NPB͒. Details on the synthesis and characterization of the PUA material were published elsewhere.6 Silicon ͑100͒ or gold-coated silicon wafer with a thickness of 100 nm using Ti ͑50 nm͒ as an adhesion promoter ͑MHS1500A metal sputter, Moohan Co., Korea͒ was used as the substrate. For a detached layer, NPB was used instead of a polymer film because of its lower cohesion energy and stability in air. 5 The thickness of NPB layer was 80-150 nm, as measured by ellipsometry ͑L116B, Gaertner, USA͒ and rms roughness was ϳ1.8 nm. To achieve conformal contact between the mold and the substrate with uniform pressure distribution, a hydraulic pressure of 0.2-2 bars was applied on the mold after inserting a thin polydimethyl siloxane ͑PDMS͒ slab as a buffer layer. While applying a pressure, temperature was increased to 90°C for 20 min on a hot plate. The glass transition temperature ͑T g ͒ of NPB is ϳ96°C. Then, the sandwiched assembly of PDMS slab and PUA mold was disintegrated after cooling to room temperature ͑cooling rate ϳ2°C/ min͒ by using a sharp tweezer. The mold was fast removed from the substrate since a high detachment rate was reported to improve the physical removal of mat...