Here's a few I would recommend:
Demon's Souls (this game has really drawn me in waaay more than I thought)
Valkyria Chronicles (if I knew then what I knew now, I would have bought a PS3 just for this game)
Any of the PixelJunk PSN games (except cars, I don't know about that one)
Shatter on PSN
Super Stardust HD
Wipeout HD (brutally hard, but a must if you like racing)
Plus the PS One classics are always hard to pass up :D
Hope this helps, and happy hunting!
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