Well alignment and overlay are use differently in projection lithography, alignment is between the mark and the mask and overlay is between different layers across the process, IDK how that would be for NIL but assuming because the absence of masks, overlay and alignment would be close related:Man the level of precision and mechanical stability you would need to get alignments consistently right at the single nanometer level is *insane*.
-An Overlay of 20nm if can be keep along the process would be like KrF level precision, good for 180-110 nm process or for metal layers.
-An Overlay of 10nm would be dry ArF precision good for backend processes and 65nm+ process
-An Overlay of 3nm would be close to Immersion and EUV, at that point because the resolution of NIL is near perfect, the sky would be the limit.