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The Vita's definitely the way to play them, too. It gives some slight but noticeable upgrades to PSP-native and PSOne-native games, including the Vita's screen itself. Especially true if you have a first-edition, OLED-screened Vita, though admittedly the 2000 feels a lot easier to hold and feels phenomenally lighter, at least to me. Still, I own a first-edition and wouldn't trade it.
One thing: Wear stereo headphones, or if you have them, studio headphones (the kind that generally has two kinds of connectors and a much longer wire). The game takes super-serious advantage of stereo headphones that adds a whole lot to the experience. The game sounds stupid-awesome on a pair of Audio-Technicas I own.
Scientists in Norway believed that they could improve the rate that leeches suck blood by dipping them in beer beforehand. That was seriously their hypothesis.