A method of patterning a substrate includes depositing an overcoat in openings of a relief pattern. The relief pattern includes a solubility-shifting agent and a deprotectable monomer sensitive to the solubility-shifting agent. The overcoat includes another deprotectable monomer sensitive to the solubility-shifting agent. The overcoat has a solubility threshold relative to a predetermined developer that is lower than the solubility threshold of the relief pattern relative to the developer. The method includes activating the solubility-shifting agent to at least reach the solubility threshold of the overcoat without reaching the solubility threshold of the relief pattern, diffusing the solubility-shifting agent a predetermined distance from structures of the relief pattern into the overcoat to form soluble regions in the overcoat, and developing the substrate with the developer to remove the soluble regions of the overcoat. The soluble regions are soluble in the developer while the relief pattern remains insoluble in the developer.