Best *atmosphere* for me is Personal Nightmare 2. And really, there hadn't been any game quite like it in terms of atmosphere until I played Scratches. Personal Nightmare still pips it though for me.
The Dark Eye is the most *unsettling*, and I absolutely love this game, it might be my favourite adventure of all time.
The scariest, of course you'd be looking at the Silent Hill and Resident Evil series'.
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