Provided herein are multi-layer stacks for use in extreme ultraviolet lithography tailored to achieve optimum etch contrast to shrink features and smooth the edges of features while enabling use of an optical leveling sensor with little or reduced error. The multi-layer stacks may include an atomically smooth layer with an average local roughness of less than a monolayer, and one or more underlayers, which may be between a target layer to be patterned and a photoresist. Also provided are methods of depositing multi-layer stacks for use in extreme ultraviolet lithography.