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I've not messed with this plugin much but after reading your post I'm thinking about giving it a whack now...If you want to use Sharpscale (i.e. don't care about fancy Adrenaline filters), change its scaling mode to literally anything other than "real." Then open up your PSP game, use the Main tab on adrenaline menu to open Official Settings, and in there uncheck the Bilinear Filtering box. You will get a razor sharp 2x integer upscale that fills the entire screen.
If you do want to use an Adrenaline scaling filter, in the adrenaline Settings tab, change graphics filtering to something other than "original" and turn smoothing to off, while leaving PSP X and Y Scale at 2.00. The LCD 3x filter and sharp bilinear are notable here for creating even more defined effects. (Note that there is an additional frame of lag using an adrenaline filter.)
The settings you pick matter more for PS1 games but let's cross that bridge when you get to it....